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1. First online X‐ray fluorescence characterization of liquid‐liquid extraction in microfluidics

Author: Jean Duhamet, Thomas Zemb, Jean-Christophe P. Gabriel, Johannes Theisen, Asmae El Maangar, Varun Rai, Fabien Olivier, Ange Maurice, Nanyang Technological University [Singapour], Université Grenoble Alpes (UGA), Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences et technologies pour une Economie Circulaire des énergies bas carbone (ISEC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Département de recherche sur les procédés pour la mine et le recyclage du combustible (DMRC), European Project: 320915,EC:FP7:ERC,ERC-2012-ADG_20120216,REE-CYCLE(2013), Nanyang Technological University (NTU), Nanyang Technological University, Energy Research Institute at NTU (ERIAN), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), CEA- Saclay (CEA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Energy Research Institute @ NTU (ERI@N), and SCARCE Laboratory
Subjects: Materials science, liquid-liquid extraction, rare earth, Microfluidics, Rare earth, Kinetics, microfluidics, Analytical chemistry, X-ray fluorescence, 02 engineering and technology, 010402 general chemistry, online x‐ray fluorescence, 01 natural sciences, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Liquid–liquid extraction, online x-ray fluorescence, [CHIM]Chemical Sciences, anisotropic interface resistance, Materials of engineering and construction. Mechanics of materials, ComputingMilieux_MISCELLANEOUS, Chemical engineering [Engineering], Anisotropic Interface Resistance, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Characterization (materials science), kinetics, TA401-492, 0210 nano-technology, liquid‐liquid extraction
Abstract: Liquid-liquid extraction is a complex chemical purification process, which is associated with many thermodynamic and kinetic values. This makes its application in the recycling industry difficult, as it deals with waste streams that have highly variable compositions. In this regard, modelling an extraction process using microfluidics proves to be a useful approach to allow rapid adaptation to such composition changes, if development can be shown to be more accurate, faster, and safer than the classical batch approach with separate analysis. Here, the first automated microfluidic tool integrated with online X-ray fluorescence (XRF) is reported to study liquid-liquid extraction processes by enabling metal concentration quantification. The measurement is automated and performed for both aqueous and organic phases to improve accuracy. Overall, this fully automated approach shows that: (i) Thermodynamic and kinetic values associated with these processes can rapidly and efficiently be obtained simultaneously (in less than 13 hours with a resulting liquid use of less than 20 mL). (ii) Numerical simulations are consistent with the experimental data and provide rare insights regarding the respective contributions to the overall kinetic of the extraction system. Ministry of National Development (MND) Ministry of the Environment and Water Resources National Environmental Agency (NEA) National Research Foundation (NRF) Published version J.C.G., O.F., A.M., V.R. acknowledge financial support from SCARCE project, which is supported by the National Research Foundation, Prime Minister’s Office, Singapore, the Ministry of National Development, Singapore, and National Environment Agency, Ministry of the Environment and Water Resource, Singapore under the Closing the Waste Loop R&D Initiative as part of the Urban Solutions & Sustainability–Integration Fund (Award No.USS-IF-2018-4). J.D., J.C.G., A.E.M., J.T, T.Z acknowledge funding from the European Research Council under the European Union’s 7th Framework Program (FP/2007-2013)/ERC Grant Agreement N◦[320915] “REE-CYCLE”: Rare Earth Element reCYCling with Low harmful Emissions.
Published: 2021

2. Impact of ionomer structuration on the performance of bio-inspired noble-metal-free fuel cell anodes

Author: Vincent Artero, Fabrice Valentino, Tristan Asset, Tran Ngoc Huan, Nathan Coutard, Bruno Jousselme, Sandrine Lyonnard, Bertrand Reuillard, Pascale Chenevier, Reuben T. Jane, Eugen S. Andreiadis, Solène Gentil, Alan Le Goff, Adina Morozan, Frédéric Maillard, Solar fuels, hydrogen and catalysis (SolHyCat), Laboratoire de Chimie et Biologie des Métaux (LCBM - UMR 5249), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Département de Chimie Moléculaire (DCM), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), ANR-17-EURE-0003,CBH-EUR-GS,CBH-EUR-GS(2017), European Project, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Subjects: Materials science, Nanotechnology, 02 engineering and technology, Carbon nanotube, engineering.material, 010402 general chemistry, 7. Clean energy, 01 natural sciences, law.invention, Catalysis, chemistry.chemical_compound, law, Nafion, Ionomer, General Environmental Science, Nanocomposite, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, Chronoamperometry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Anode, chemistry, engineering, General Earth and Planetary Sciences, Noble metal, 0210 nano-technology
Abstract: https://www.sciencedirect.com/science/article/pii/S2667109321000014?via%3Dihub; International audience; Molecular-engineered bio-inspired catalysts hold promise for the next generation of proton-exchange membrane fuel cells (PEMFCs). Yet, their implementation in catalytic layers with Nafion ionomer faces nanocomposite formulation issues. Here, we use various DuBois nickel catalysts immobilized on carbon nanotubes to exemplify how self-assembly at the mesoscale affects H2 oxidation anode performance. We exploited the reversible activity of these catalysts together with potential-step chronoamperometry to locally produce H2 and probe mass transport within the catalyticlayer. Small-angle neutron scattering studies serve to build a model describing how the surface functionalization drives the structuration of the ionomer and affects the diffusion of protons and gas from and to catalytic centers. This study thus demonstrates that implementation of unconventional catalysts in catalytic layers requires the redesign of the whole system of materials. On the basis of such information, catalytic layer formulation was optimized,allowing order-of-magnitude performance enhancement of noble-metal-free PEMFCs
Published: 2021

3. Review on modelling of corrosion under droplet electrolyte for predicting atmospheric corrosion rate

Author: Yves Van Ingelgem, Mesfin Haile Mamme, Bangalore Gangadharacharya Koushik, Herman Terryn, Nils Van den Steen, Faculty of Engineering, Materials and Chemistry, Electrochemical and Surface Engineering, and Materials and Surface Science & Engineering
Subjects: Materials science, Polymers and Plastics, Condensation, Evaporation, 02 engineering and technology, Electrolyte, 010402 general chemistry, 01 natural sciences, Corrosion, Cathodic protection, Materials Chemistry, Relative humidity, Diffusion (business), Mathematical modelling, Mechanical Engineering, Metals and Alloys, Water droplets, 021001 nanoscience & nanotechnology, 6. Clean water, 0104 chemical sciences, Chemical engineering, 13. Climate action, Mechanics of Materials, Ceramics and Composites, Limiting oxygen concentration, Atmospheric corrosion, 0210 nano-technology
Abstract: Atmospheric corrosion of metals is the most common type of corrosion which has a significant impact on the environment and operational safety in various situations of everyday life. Some of the common examples can be observed in land, water and air transportation systems, electronic circuit boards, urban and offshore infrastructures. The dew drops formed on metal surface due to condensation of atmospheric moisture facilitates corrosion as an electrolyte. The corrosion mechanisms under these droplets are different from classically known bulk electrolyte corrosion. Due to thin and non-uniform geometric thickness of the droplet electrolyte, the atmospheric oxygen requires a shorter diffusion path to reach the metal surface. The corrosion under a droplet is driven by the depletion of oxygen in the center of the droplet compared to the edge, known as differential aeration. In case of a larger droplet, differential aeration leads to preferential cathodic activity at the edge and is controlled by the droplet geometry. Whereas, for a smaller droplet, the oxygen concentration remains uniform and hence cathodic activity is not controlled by droplet geometry. The geometry of condensed droplets varies dynamically with changing environmental parameters, influencing corrosion mechanisms as the droplets evolve in size. In this review, various modelling approaches used to simulate the corrosion under droplet electrolytes are presented. In the efforts of developing a comprehensive model to estimate corrosion rates, it has been noted from this review that the influence of geometric evolution of the droplet due to condensation/evaporation processes on corrosion mechanisms are yet to be modelled. Dynamically varying external factors like environmental temperature, relative humidity, presence of hygroscopic salts and pollutants influence the evolution of droplet electrolyte, making it a complex phenomenon to investigate. Therefore, an overview of available dropwise condensation and evaporation models which describes the formation and the evolution of droplet geometry are also presented from an atmospheric corrosion viewpoint.
Published: 2021

4. A highly efficient solution and solid state ESIPT fluorophore and its OLED application

Author: Pei Yu, Sophie Gadan, Sandra Mazerat, Bernard Geffroy, Gilles Clavier, Anne Léaustic, Clémence Allain, Virgile Trannoy, Régis Guillot, Institut de Chimie Moléculaire et des Matériaux d'Orsay (ICMMO), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), ANR-11-IDEX-0003,IPS,Idex Paris-Saclay(2011), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Fluorophore, Proton, 010405 organic chemistry, Chemistry, Hydrogen bond, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Electroluminescence, 010402 general chemistry, 01 natural sciences, Fluorescence, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, Crystallography, Intramolecular force, Excited state, Materials Chemistry, OLED
Abstract: We present herein the synthesis and the photophysics of 2,2’-bipyridine-3,3’-diol-5,5’-dicarboxylic acid ethyl ester (BP(OH)$_2$DCEt$_2$), an excited state intramolecular proton tranfer (ESIPT)-based fluorophore featuring two identical intramolecular hydrogen bonds. BP(OH)$_2$DCEt$_2$ emits efficiently not only in solution, including protic solvents ($\lambda _{em}$ = 521 nm, $\Phi$$_f$ = 40 to 75%), but also in crystalline state ($\lambda _{em}$ = 530 nm, $\Phi$$_f$ = 51%). In addition, its saponified form (Na2BP(OH)2DC) is highly fluorescent in water ($\lambda _{em}$ = 490 nm, $\Phi$$_f$ = 51%). Finally, the good electroluminescence performance of BP(OH)$_2$DCEt$_2$ is also demonstrated in an OLED device.
Published: 2021
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5. Local probe investigation of electrocatalytic activity

Author: A. Boudet, R. Cornut, N. Limani, Bruno Jousselme, N. Blanchard, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), European Project: 812398,SENTINEL, European Project: 779550,PEGASUS, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, business.industry, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrocatalyst, 7. Clean energy, 01 natural sciences, Electrochemical energy conversion, 0104 chemical sciences, Renewable energy, Chemistry, Scanning electrochemical microscopy, Scanning probe microscopy, 13. Climate action, Fuel cells, 0210 nano-technology, business
Abstract: As the world energy crisis remains a long-term challenge, development and access to renewable energy sources are crucial for a sustainable modern society. Electrochemical energy conversion devices are a promising option for green energy supply, although the challenge associated with electrocatalysis have caused increasing complexity in the materials and systems, demanding further research and insights. In this field, scanning probe microscopy (SPM) represents a specific source of knowledge and understanding. Thus, our aim is to present recent findings on electrocatalysts for electrolysers and fuel cells, acquired mainly through scanning electrochemical microscopy (SECM) and other related scanning probe techniques. This review begins with an introduction to the principles of several SPM techniques and then proceeds to the research done on various energy-related reactions, by emphasizing the progress on non-noble electrocatalytic materials., Investigation of electrocatalytic materials with scanning probe techniques (SECM, SICM, SECCM and AFM) for energy storage and conversion devices.
Published: 2021
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6. Steady‐State Electrocatalytic Activity Evaluation with the Redox Competition Mode of Scanning Electrochemical Microscopy: A Gold Probe and a Boron‐Doped Diamond Substrate

Author: Alice Boudet, Olivier Henrotte, Renaud Cornut, Bacem Zribi, Ndrina Limani, Emmanuel Scorsone, Bruno Jousselme, Philippe Bergonzo, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Capteurs Diamant (LCD-LIST), Département Métrologie Instrumentation & Information (DM2I), Laboratoire d'Intégration des Systèmes et des Technologies (LIST), Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire d'Intégration des Systèmes et des Technologies (LIST), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, University College of London [London] (UCL), European Project: 812398,SENTINEL, European Project: 779550,PEGASUS, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Intégration des Systèmes et des Technologies (LIST (CEA)), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire d'Intégration des Systèmes et des Technologies (LIST (CEA))
Subjects: Materials science, chemistry.chemical_element, Nanotechnology, Context (language use), substrate, probe, 02 engineering and technology, engineering.material, 010402 general chemistry, Electrochemistry, Electrocatalyst, 01 natural sciences, Catalysis, redox competition scanning electrochemical microscopy (RC‐SECM), Scanning electrochemical microscopy, diamond, steady‐state measurement, boron‐doped diamond, [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], instrumentation, oxygen reduction reaction, detector, Substrate (chemistry), Diamond, [CHIM.MATE]Chemical Sciences/Material chemistry, gold, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], engineering, 0210 nano-technology, Platinum, catalyst
Abstract: International audience; In the current context of energetic transition, investigations of alternative complex systems require tools such as scanning electrochemical microscopy (SECM), offering interesting opportunities as an electroanalytical technique to evaluate innovative catalysts. Herein, we demonstrate how a judicious choice of probe and substrate materials opens up improved performances to achieve steady‐state measurements for oxygen reduction reaction (ORR) catalytic activity detection through redox competition scanning electrochemical microscopy (RC‐SECM). On the probe side, we show that using gold enhances the stability of the local oxygen concentration detection in comparison to the regularly used platinum one. On the substrate side, we evaluate boron‐doped diamond as an appealing alternative to classical support substrate, that shows a low ORR activity, high stability and very good reusability. This work introduces an alternative approach for quantitative measurements with SECM, improving measurement ease, comfort and reproducibility, thus paving the way towards standardized benchmarking and numerical simulation‐based parameter extraction.
Published: 2020

7. Direct reuse of electronic plastic scraps from computer monitor and keyboard to direct stem cell growth and differentiation

Author: Jean-Christophe P. Gabriel, Jong-Min Lee, Zhuoran Wu, Chor Yong Tay, Pujiang Shi, Madhavi Srinivasan, Chiew Kei Tan, Nanyang Technological University [Singapour], Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), School of Chemical & Biomedical Engineering, National Research Foundation, Singapore, and National Environment Agency, Singapore under its Closing the Waste Loop Funding Initiative (Award No. USS-IF-2018-4), Project 'NTU Singapore –CEA Alliance for Research in Circular Economy (SCARCE) - Research Thrust 4', Nanyang Technological University, Energy Research Institute at NTU (ERIAN), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), School of Materials Science and Engineering, School of Biological Sciences, 'NTU Singapore –CEA Alliance for Research in Circular Economy (SCARCE)', School of Chemical and Biomedical Engineering, and Energy Research Institute @ NTU (ERI@N)
Subjects: Environmental Engineering, business.product_category, Materials science, Waste Valorization, Cellular differentiation, Nanotechnology, 02 engineering and technology, Substrate (printing), Reuse, 010402 general chemistry, 01 natural sciences, Contact guidance, 12. Responsible consumption, chemistry.chemical_compound, Osteogenesis, Humans, Environmental Chemistry, Diffuser (sewage), Waste Management and Disposal, Waste management, Materials [Engineering], Computers, Acrylonitrile butadiene styrene, Stem Cells, Cell Differentiation, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Pollution, Waste valorization, 0104 chemical sciences, Electronic-plastics, chemistry, Stem cell differentiation, Cell culture, Electronics, Computer monitor, Stem cell, 0210 nano-technology, business, Plastics, Electronic-Plastics
Abstract: Reuse of electronic wastes is a critical aspect for a more sustainable circular economy as it provides the simplest and most direct route to extend the lifespan of non-renewable resources. Herein, the distinctive surface and micro topographical features of computer electronic-plastic (E-plastic) scraps were unconventionally repurposed as a substrate material to guide the growth and differentiation of human adipose-derived mesenchymal stem cells (ADSCs). Specifically, the E-plastics were scavenged from discarded computer components such as light diffuser plate (polyacrylates), prismatic sheet (polyethylene terephthalate), and keyboards (acrylonitrile butadiene styrene) were cleaned, sterilized, and systematically characterized to determine the identity of the plastics, chemical constituents, surface features, and leaching characteristics. Multiparametric analysis revealed that all the E-plastics could preserve stem-cell phenotype and maintain cell growth over 2 weeks, rivalling the performance of commercial tissue-culture treated plates as cell culture plastics. Interestingly, compared to commercial tissue-culture treated plastics and in a competitive adipogenic and osteogenic differentiation environment, ADSCs cultured on the keyboard and light diffuser plastics favoured bone cells formation while the grating-like microstructures of the prismatic sheet promoted fat cells differentiation via the process of contact guidance. Our findings point to the real possibility of utilizing discarded computer plastics as a "waste-to-resource" material to programme stem cell fate without further processing nor biochemical modification, thus providing an innovative second-life option for E-plastics from personal computers. National Environmental Agency (NEA) National Research Foundation (NRF) This research is supported by the National Research Foundation, Singapore, and National Environment Agency, Singapore under its Closing the Waste Loop Funding Initiative (Award No. USS-IF-2018-4).
Published: 2022

8. Studying Chemisorption at Metal–Polymer Interfaces by Complementary Use of Attenuated Total Reflection–Fourier Transform Infrared Spectroscopy (ATR-FTIR) in the Kretschmann Geometry and Visible–Infrared Sum-Frequency Generation Spectroscopy (SFG)

Author: Huib J. Bakker, Jan Versluis, L.I. Fockaert, Johannes M. C. Mol, Deborah Ganzinga-Jurg, B. Boelen, Herman Terryn, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: Nonlinear optics, Materials science, Infrared, Interfaces, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, Zinc, 010402 general chemistry, 01 natural sciences, stomatognathic system, Physical and Theoretical Chemistry, Fourier transform infrared spectroscopy, Organic polymers, Oxides, Molecular configuration, 021001 nanoscience & nanotechnology, Infrared light, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, chemistry, Chemisorption, Attenuated total reflection, 0210 nano-technology, Sum frequency generation spectroscopy
Abstract: The molecular configuration and chemistry at the zinc/zinc oxide-polyester interface were studied by using two complementary spectroscopic techniques: attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR) and sum-frequency generation (SFG) spectroscopy. It was shown that ATR-FTIR should be considered as a (3D) interphase-sensitive technique with probing depths of 250-400 nm in the headgroup region (2000-1200 cm-1). On the other hand, SFG is known to be a (2D) interface-sensitive technique. The ATR-FTIR measurements showed that carboxylate groups are formed within the near-interface region of the polyester phase. SFG measurements showed that the carboxylic acid groups are stable at the polymer-zinc/zinc oxide interface. In addition, in situ ATR-FTIR and SFG measurements have been conducted when exposing the polyester-zinc/zinc oxide system to D2O. The exposure to D2O is observed to lead to an additional conversion of ester and carboxylic acid groups to carboxylate groups. The comparison of the SFG and ATR-FTIR measurements shows that this conversion occurs much slower at the polyester-zinc/zinc oxide interface than in the bulk of the polyester. Finally, the strengths and limitations as well as the complementarity of both techniques are discussed.
Published: 2020

9. Naphthyl‐Fused Phosphepines: Luminescent Contorted Polycyclic P‐Heterocycles

Author: Denis Tondelier, Thomas Delouche, Thierry Roisnel, Zoltán Benkő, Pierre-Antoine Bouit, Réka Mokrai, Bernard Geffroy, Muriel Hissler, László Nyulászi, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Budapest University of Technology and Economics [Budapest] (BME), 16-CE05-0003-01, 17-CE09-0020, Agence Nationale de la Recherche, ANR-17-CE09-0020,FluoHyb,Nouveaux matériaux hybrides fluorescents basés sur le concept de l'émission induite par agrégation de chromophores organiques greffés sur des nanoparticules inorganiques.(2017), ANR-16-CE05-0003,Heterographene,Synthèse et étude des propriétés électroniques de polycycles aromatiques contenant des hétéroatomes(2016), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and MTA-BME Research Group of Technical Analytical Chemistry
Subjects: optical properties, Steric effects, Substitution reaction, [CHIM.ORGA]Chemical Sciences/Organic chemistry, 010405 organic chemistry, Organic Chemistry, Oxide, P-heterocycles, General Chemistry, organic light-emitting diodes, pi-conjugated systems, 010402 general chemistry, Photochemistry, 01 natural sciences, Redox, Catalysis, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry.chemical_compound, chemistry, OLED, Cyclic voltammetry, Luminescence, density function calculations, Pnictogen
Abstract: International audience; This article presents the synthesis of a new family of naphthyl-fused phosphepines through Ni-mediated C-C coupling. Interestingly, the chlorophosphine oxide intermediate shows strong resistance toward oxidation/hydrolysis owing to a combination of steric hindrance and pnictogen interactions. However, it can undergo substitution reactions under specific conditions. The optical/redox properties and the electronic structure of these new π-systems were studied experimentally (UV/Vis absorption, emission, cyclic voltammetry) and computationally (TD-DFT calculations, NICS investigation). Taking advantage of the luminescence of these derivatives, a blue-emitting OLED has been prepared, highlighting that these novel π-conjugated P-heterocycles appear to be promising building blocks for solid-state lighting applications.
Published: 2020

10. Reversible densification in nano-Li2MnO3 cation disordered rock-salt Li-ion battery cathodes

Author: Yves Joly, Maria Diaz-Lopez, Olivier Proux, Valerie Pralong, Pierre Bordet, Philip A. Chater, Jean-Louis Hazemann, DIAMOND Light source, ISIS Neutron and Muon Source (ISIS), STFC Rutherford Appleton Laboratory (RAL), Science and Technology Facilities Council (STFC)-Science and Technology Facilities Council (STFC), Surfaces, Interfaces et Nanostructures (SIN), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), European Synchrotron Radiation Facility (ESRF), Matériaux, Rayonnements, Structure (MRS), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC), Surfaces, Interfaces et Nanostructures (NEEL - SIN), Matériaux, Rayonnements, Structure (NEEL - MRS), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Extended X-ray absorption fine structure, Renewable Energy, Sustainability and the Environment, Scattering, Analytical chemistry, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, XANES, Cathode, 0104 chemical sciences, Ion, law.invention, law, Nano, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Materials Science, Neutron, 0210 nano-technology
Abstract: International audience; The full structure of nano-Li 2 MnO 3 with superior reversible capacities of 290 mA h g À1 for over 10 cycles was investigated by neutron and X-ray total scattering, which demonstrate that contrary to previous claims, a phase transformation occurs during synthesis forming a disordered cubic MnO-type rock-salt with nanodomains of Li/Mn layering of $1 nm. A comprehensive study of the structural and charge evolution combining in operando X-ray total scattering with advanced spectroscopic methods at the Mn K-edge such as High Energy Resolved Fluorescence Detected XANES, EXAFS and Emission Spectroscopies including main and valence-to-core transitions, point to a lattice densification with an effective loss of Li 2 O, with the subsequent electrochemical activation of Li 2 O as the main responsible mechanism for the exchanged capacity. Interestingly, and unlike previous studies, no capacity losses could be associated to the material's densification.
Published: 2020

11. One‐step Preparation of Fe/N/C Single‐atom Catalysts Containing Fe−N4 Sites from an Iron Complex Precursor with 5,6,7,8‐Tetraphenyl‐1,12‐diazatriphenylene Ligands

Author: Masaru Kato, Ichizo Yagi, Stephane Campidelli, Shin Ichiro Noro, Takashi Hayashi, Norimitsu Tohnai, Kiyotaka Asakura, Akira Onoda, Siqi Xie, Koki Matsumoto, Graduate School of Engineering, Osaka University, Graduate School of Engineering, Graduate School of Environmental Science, Hokkaido University, Hokkaido University [Sapporo, Japan], institute of catalysis, Hokkaido University of Science, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), JSPS KAKENHI Grant Numbers 25708031, JP15H03857, JP15H05804, and JP19K22202, JP19H04579, and the Iketani Science and Technology Foundation., Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: X-ray absorption spectroscopy, Absorption spectroscopy, 010405 organic chemistry, Chemistry, Organic Chemistry, Aromaticity, General Chemistry, Carbon black, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, Electrochemistry, 01 natural sciences, Redox, Catalysis, 0104 chemical sciences, Polymer chemistry, Pyrolysis
Abstract: International audience; Fe/N/C single-atom catalysts containing Fe−N x sites prepared by pyrolysis are promising cathode materials for fuel cells and metal-air batteries due to their high oxygen reduction reaction (ORR) activities. We have developed iron complexes containing N2- or N3-chelating coordination structures with preorganized aromatic rings in a 1,12-diazatriphenylene framework tethering bromo substituents as precursors to precisely construct Fe−N 4 sites in an Fe/N/C catalyst. One-step pyrolysis of the iron complex with carbon black forms atomically dispersed Fe−N 4 sites without iron aggregates. X-ray absorption spectroscopy (XAS) and electrochemical measurements revealed that the iron complex with N3-coordination is more effectively converted to Fe−N 4 sites catalyzing ORR with a TOF value of 0.21 e∙site −1 ∙s −1 at 0.8 V vs RHE. This indicates that the formation of Fe−N 4 sites is controlled by precise tuning of the chemical structure of the iron complex precursor.
Published: 2022

12. Si-containing Polycyclic Aromatic Hydrocarbons: Synthesis and Opto-electronic Properties

Author: Payal Manzhi, Bernard Geffroy, Marie Cordier, Ghizlene Taifour, Denis Jacquemin, Boris Le Guennic, Muriel Hissler, Thomas Delouche, Pierre-Antoine Bouit, Denis Tondelier, Thierry Roisnel, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Chimie Et Interdisciplinarité : Synthèse, Analyse, Modélisation (CEISAM), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Heterographene ANR-16-CE05-0003-01, Agence Nationale de la Recherche, and ANR-16-CE05-0003,Heterographene,Synthèse et étude des propriétés électroniques de polycycles aromatiques contenant des hétéroatomes(2016)
Subjects: Organic electronics, Materials science, 010405 organic chemistry, business.industry, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Metals and Alloys, General Chemistry, Electroluminescence, 010402 general chemistry, 01 natural sciences, Redox, Catalysis, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Materials Chemistry, Ceramics and Composites, Optoelectronics, Opto electronic, business, Luminescence
Abstract: International audience; We report a straightforward synthesis of Si-containing Polycyclic Aromatic Hydrocarbons (PAHs). The impact of π-extension and exocyclic modifications on both the optical and redox properties is investigated using a joint experimental/theoretical approach. By taking advantage of the solid-state luminescence of these derivatives, electroluminescent devices are prepared. Such preliminary opto-electronic results highlight that these heteroatom-containing PAHs are promising building blocks for organic electronics.
Published: 2022

13. Experimental determination of the curvature-induced intra-wall polarization of inorganic nanotubes

Author: Sophie Le Caër, Aleksandar R. Milosavljević, Olivier Sublemontier, Jean Philippe Renault, Sabyasachi Patra, Antoine Thill, Jocelyne Leroy, Christophe Nicolas, Lucie Huart, Marie-Claire Pignié, Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Laboratoire Edifices Nanométriques (LEDNA), CEA Bottom Up 2020-21 grant: project PHOTOTUBE, Ile de France DIM RESPORE 2019-20 and CEA Bottom Up 2020-21 grants funded this study by the project GRANITE, ANR-20-CE09-0029,BENALOR,Imogolites hybrides comme réacteur modulable(2020), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685)
Subjects: Nanotube, Materials science, Valence (chemistry), Diffuse reflectance infrared fourier transform, Doping, Imogolite, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, 0104 chemical sciences, X-ray photoelectron spectroscopy, Chemical engineering, Photocatalysis, Water splitting, General Materials Science, 0210 nano-technology
Abstract: Inspired by a natural nano-mineral known as imogolite, aluminosilicate inorganic nanotubes are appealing systems for photocatalysis. Here, we studied two types of synthetic imogolites: one is completely hydrophilic (IMO-OH), while the other has a hydrophilic exterior and a hydrophobic interior (IMO-CH3), enabling the encapsulation of organic molecules. We combined UV-Vis diffuse reflectance spectroscopy of imogolite powders and X-ray photoelectron spectroscopy of deposited imogolite films and isolated nanotubes agglomerates to obtain not only the band structure, but also the quantitative intra-wall polarization of both synthetic imogolites for the first time. The potential difference across the imogolite wall was determined to be 0.7 V for IMO-OH and around 0.2 V for IMO-CH3. The high curvature of the nanotubes, together with the thinness of their wall, favors efficient spontaneous charge separation and electron exchange reactions on both the internal and external nanotube surfaces. In addition, the positions of their valence and conduction band edges make them interesting candidates for co-catalysts or doped catalysts for water splitting, among other possible photocatalytic reactions relevant to energy and the environment.
Published: 2021
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14. Reversible Photo-Induced Phase Segregation and Origin of Long Carrier Lifetime in Mixed-Halide Perovskite Films

Author: Bernard Geffroy, Douglas R. Miquita, Olivier Plantevin, Minjin Kim, Subodh K. Gautam, Jean-Eric Bourée, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Centro de Microscopia, Universidade Federal de Minas Gerais [Belo Horizonte] (UFMG), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and ANR-16-CE05-0019,PERSIL,Cellules solaires tandem Perovskite-Silicium nanocristallin(2016)
Subjects: Photoluminescence, Materials science, Band gap, FOS: Physical sciences, 02 engineering and technology, Applied Physics (physics.app-ph), 010402 general chemistry, 7. Clean energy, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, Biomaterials, [SPI]Engineering Sciences [physics], Phase segregation, Phase (matter), Electrochemistry, [CHIM.CRIS]Chemical Sciences/Cristallography, Hybrid perovskite, Perovskite (structure), [PHYS]Physics [physics], Condensed Matter - Materials Science, business.industry, Materials Science (cond-mat.mtrl-sci), Carrier lifetime, Triple-cation mixed-halide perovskite, [CHIM.MATE]Chemical Sciences/Material chemistry, Physics - Applied Physics, Exciton-phonon coupling, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Long carrier lifetime, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Photoexcitation, Semiconductor, Chemical physics, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Charge carrier, 0210 nano-technology, business
Abstract: International audience; Mixed-halide based hybrid perovskite semiconductors have attracted tremendous attention as a promising candidate for high efficient photovoltaic and light-emitting devices. However, these advanced perovskite materials may undergo phase segregation under light illumination due to halide ion migration, affecting their optoelectronic properties. Here, we report photo-excitation induced phase segregation in triple-cation mixed-halide perovskite films that yields to red-shift in photoluminescence response. We demonstrate that photo-excitation induced halide ion migration leads to the formation of smaller-bandgap iodide-rich and larger-bandgap bromide-rich domains in the perovskite film, where the phase segregation rate is found to follow the excitation power-density as a power law. Results confirm that charge carrier lifetime increases with redshift in photoluminescence due to the trapping of photo-excited carriers in the segregated smaller-bandgap iodide-rich domains. Interestingly, we found that these photo-induced changes are fully reversible and thermally activated when the excitation power is turned off. A significant difference in activation energies for halide ion migration is observed during phase segregation and recovery process under darkness. Additionally, we have investigated the emission linewidth broadening as a function of temperature which is governed by the exciton-optical phonon coupling. The mechanism of photo-induced phase segregation is interpreted based on excitonphonon coupling strength in both mixed and demixed (segregated) states of perovskite film.
Published: 2021

15. Tuning the Aggregation Behaviour of BN-Coronene Diimides with the Imide Substituents and their Performance in Devices (OLED, OFET)

Author: Anne Staubitz, Jonas Hoffmann, Bernard Geffroy, Emmanuel Jaques, Muriel Hissler, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Bremen, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut d'Électronique et des Technologies du numéRique (IETR), Université de Nantes (UN)-Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique, CM 1302 (SIPS), European Cooperation in Science and Technology, STA1195/2-1, Deutsche Forschungsgemeinschaft, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Nantes Université (NU)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), Université de Rennes 1 (UR1), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université de Nantes (UN)-Université de Rennes 1 (UR1)
Subjects: Materials science, 010405 organic chemistry, [CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemistry, 010402 general chemistry, Photochemistry, 01 natural sciences, Coronene, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Bathochromic shift, Materials Chemistry, OLED, Hypsochromic shift, Molecular orbital, Luminescence, Imide, Perylene
Abstract: International audience; Compared to perylene diimides (PDIs), the coronene diimides (CDIs), which can be viewed as a lateral core extension, show undesired effects for optoelectronic devices such as the decrease of the absorption and a hypsochromic shift. Here, we demonstrate that if the core is extended with two BN units as opposed to two CC units, the opposite is true: Large bathochromic shifts can be achieved, together with higher molar extinction coefficients and beneficial luminescence properties, e.g. a small Stokes shift and high quantum yields (lum >94%). These effects can be explained by the influence of the BN-unit onto the frontier molecular orbitals of the BNCDI. Different substitution motifs at the imide-position, cylcohexyl and 2,6-diisopropylphenyl, although they had no influence on the optical properties on a single molecule level, influenced the aggregation substantially so that the optical properties in the solid-state and the performance in organic devices (OLED and OFET) differed considerably. In combination with host matrices devices with EQE up to 1.5% and white light emission (0.317; 0.346) were obtained. The developed synthetic route starting from a regioisomeric pure 1,7substituted PDI leads to BNCDIs in good yields, which makes this class of compounds very promising.
Published: 2021
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16. Highly emissive layers based on organic/inorganic nanohybrids using Aggregation Induced Emission effect

Author: Olivier Margeat, Meriem Gaceur, Mathieu Denis, Muriel Hissler, Matthew P. Duffy, Bernard Geffroy, Xianjie Liu, Qinye Bao, Thomas Dombray, Yahia Didane, Jörg Ackermann, Alessandro Mattoni, Mats Fahlman, Pietro Delugas, Nicolas Ledos, Pierre-Antoine Bouit, Jonathan Phelipot, Denis Tondelier, Ting Wang, Centre Interdisciplinaire de Nanoscience de Marseille (CINaM), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Linköping University (LIU), CNR Istituto Officina dei Materiali (IOM), Consiglio Nazionale delle Ricerche [Roma] (CNR), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), This work is supported by the Ministère de la Recherche et de l'Enseignement Supérieur, the CNRS, the Région Bretagne (ARED grant to NL), the French National Research Agency (ANR Fluohyb ANR-17-CE09-0020) and the SATT Sud-Est. The authors thank T. Roisnel (CDifX, ISCR) for X-ray diffraction analysis and A.Ranguis (CINaM) for AFM measurements. A.M. acknowledges MUR for project PON04a2 00490 M2M Netergit and PRACEfor awarding access to Marconi KNL at CINECA, Italy, through project PROVING-IL (2019204911)., ANR-17-CE09-0020,FluoHyb,Nouveaux matériaux hybrides fluorescents basés sur le concept de l'émission induite par agrégation de chromophores organiques greffés sur des nanoparticules inorganiques.(2017), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS)
Subjects: Fluorophore, Materials science, Nanoparticle, 02 engineering and technology, 010402 general chemistry, Photochemistry, 01 natural sciences, hydroxyoxoposphole, Industrial and Manufacturing Engineering, AIE, chemistry.chemical_compound, X-ray photoelectron spectroscopy, hybrid materials, OLED, General Materials Science, Thin film, [CHIM.ORGA]Chemical Sciences/Organic chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Fluorescence, 0104 chemical sciences, chemistry, Mechanics of Materials, Intramolecular force, nanoparticles, fluorescence, 0210 nano-technology, Hybrid material
Abstract: International audience; Fluorescent nanohybrids, based on p-extended hydroxyoxophosphole ligands grafted onto ZnO nanoparticles, were designed and studied. The restriction of the intramolecular motions of the organic fluorophore, through either aggregates' formation in solution or processing into thin films, forms highly emissive materials due to a strong Aggregation Induced Emission effect. Theoretical calculations and XPS analyses were performed to analyze the interactions between the organic and inorganic counterparts. Preliminary results on the use of these nanohybrids as solution-processed emissive layers in Organic Light Emitting Diodes (OLEDs) illustrate their potential for lighting applications.
Published: 2021

17. Li leaching from Li carbonate-primer

Author: Herman Terryn, Pieter Visser, A.M. Glenn, S. Ranade, Jamie S. Laird, Anthony E. Hughes, Johannes M. C. Mol, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: characterisation, Lithium inhibitor, Void (astronomy), Materials science, Ion beam, General Chemical Engineering, Analytical chemistry, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, Metal, Depletion region, Materials Chemistry, Porosity, Dissolution, Primer (paint), Organic Chemistry, coating, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Corrosion, visual_art, engineering, visual_art.visual_art_medium, Leaching, Chemical Engineering(all), Leaching (metallurgy), 0210 nano-technology
Abstract: Depletion depths of inorganic components from a scribe edge in a polyurethane primer containing Li2CO3, MgO, BaSO4 and TiO2 beneath a topcoat, were determined using a range of techniques including SEM/EDS and proton induced X-ray and γ-ray emission spectroscopies. SEM of sections cut using an ion beam revealed scribe damage penetrating 20–25 μm away from the scribe edge prior to leaching. After neutral salt spray (NSS) exposure a leached zone developing from the scribe edge was observed. For longer NSS exposure times (>96 h) this leached zone of nearly complete Li and Mg depletion did not develop any deeper than the scribe damaged region indicating that the depletion zone was caused by mechanical damage due to scribing. At short times small voids were formed in Li2CO3 particles within the primer well away from the scribe (100–260 μm) whereas a mixture of void and detachment in and around Li2CO3 particles was observed at longer times. The detachment was assumed to be part of a channel network within clusters of particles. Internal stresses within the primer resulting from buildup of inhibitor dissolution product within the voids were modelled using finite element analysis. It was found that strains related to von Mises stresses were concentrated around the inorganic particles and developed preferentially within the plane of the primer beneath the topcoat with some indication of concentration towards the primer/metal interface. These stresses resulted from osmosis and swelling related to the voids. They were also attributed to the observed cracking of the binder at some locations. Leaching experiments showed that Li was released very rapidly from the primer. The leaching data was modelled using a power law where the mass released is proportional to tn where the n is an index that reflects the kinetic behavior dictated by the evolving primer porosity. In this study n values between 0 and 1 were observed for all species, with Li starting at around 0.7 but rapidly decreasing to close to zero.
Published: 2021

18. Hole injection from P1 dye hot-excited states in p-type dye-sensitized films: a fluorescence study

Author: Bruno Jousselme, Thomas Gustavsson, Valentin Maffeis, Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), CEA-DSM Energie program (PHLUMVIR project), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Relaxation (NMR), [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, Fluorescence, Photon upconversion, 0104 chemical sciences, 3. Good health, Electron transfer, Picosecond, Excited state, Femtosecond, Physical and Theoretical Chemistry, Time-resolved spectroscopy, 0210 nano-technology
Abstract: International audience; We present a study of the excited state relaxation dynamics of the photosensitizer P1 used in p-type dye-sensitized solar cells. Comparative femtosecond fluorescence upconversion measurements in solution and in films show that the dye undergoes a picosecond electronic relaxation from the bright Franck–Condon (FC) state to a low-emitting charge-transfer (CT) state in polar environment. The fluorescence is moderately quenched in solution and on the mesoporous Al2O3 isolator but dramatically more on NiO semiconductor. We assign this sub-picosecond process to the hole injection thus confirming that the electron transfer is from the FC state directly into the NiO valence band.
Published: 2021

19. 2D Monolayer of 1T' Phase of Alloyed WSSe from Colloidal Synthesis

Author: Abdelkarim Ouerghi, Benoit Mahler, Ashkan Shahmanesh, Corentin Dabard, Julien Chaste, Charlie Gréboval, Mathieu G. Silly, Matteo Calandra, Matthieu Bugnet, Davide Romanin, Debora Pierucci, Christophe Méthivier, Emmanuel Lhuillier, Sang-Soo Chee, Luminescence (LUMINESCENCE), Institut Lumière Matière [Villeurbanne] (ILM), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon, Spectroscopie des nouveaux états quantiques (INSP-E2), Institut des Nanosciences de Paris (INSP), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et d'Etude des Matériaux (UMR 8213) (LPEM), Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Physico-chimie et dynamique des surfaces (INSP-E6), Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Matériaux, ingénierie et science [Villeurbanne] (MATEIS), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), University of Trento [Trento], ANR-19-CE09-0017,FRONTAL,Nanocristaux Colloïdaux Dopés Infrarouges(2019), ANR-19-CE24-0022,COPIN,Détecteur plasmonique à nanoCristaux colloïdaux: une nouvelle filière pour l'OPtoélectronique INfrarouge(2019), ANR-19-CE09-0026,GRaSkop,Tuning Giant Rashba Spin-Orbit Coupling in Polar Single Layer Transition Metal Dichalcogenides(2019), ANR-18-CE30-0023,IPER-Nano2,Nanocristaux de perovskite inorganique pour la nanophotonique(2018), ANR-10-LABX-0067,MATISSE,MATerials, InterfaceS, Surfaces, Environment(2010), ANR-20-ASTR-0008,NITquantum,Design et fabrication d'un plan focal dans le proche infrarouge à base de nanocrisrtaux(2020), European Project: 756225,blackQD, and Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, 2D monolayer, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Transition metal dichalcogenides, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Condensed Matter::Materials Science, General Energy, Chemical engineering, Phase (matter), Monolayer, Physical and Theoretical Chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 0210 nano-technology, Raman, Photoemission, Density Functional Theory, Colloidal synthesis
Abstract: International audience; We explore the colloidal growth of monolayers of WSSe alloy in their 1T' phase with various Se content. We develop a synthetic procedure leading to reduced aggregation of the flakes. The presence of a narrow band-gap close to the top of the valence band has been evidenced combining photoemission spectroscopy and density functional theory (DFT). The electronic structure is weakly affected by the variation of the alloy content and atomic ordering. µ-Raman spectroscopy and STEM are used to confirm the obtained 1T' phase, while simulations of the Raman spectra suggest contribution from both the S and Se atoms in the Raman spectra. Finally, we use electronic transport and photoconduction and reveal a short coherence length consistent with the defective nature of the flakes.
Published: 2021

20. Redox-Triggered Control of Cell Adhesion and Deadhesion on Poly(lysine)-g-poly(ethylene oxide) Adlayers

Author: Simon de Beco, Julien Dupré de Baubigny, Vincent Humblot, Pierre Lalanne, Catherine Villard, Mathieu Coppey, Christophe Tribet, Emmanuelle Marie, Louise Hespel, Processus d'Activation Sélective par Transfert d'Energie Uni-électronique ou Radiatif (UMR 8640) (PASTEUR), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Physico-Chimie-Curie (PCC), Centre National de la Recherche Scientifique (CNRS)-Institut Curie [Paris]-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC), Laboratoire Physico-Chimie Curie [Institut Curie] (PCC), Institut Curie [Paris]-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-11-LABX-0011,DYNAMO,Dynamique des membranes transductrices d'énergie : biogénèse et organisation supramoléculaire.(2011), ANR-17-CE09-0019,CASCADE,Contrôle de l'accessibilité de ligands dans le temps et dans l'espace sur des surfaces nanopatternées pour l'adhésion cellulaire(2017), Polymères Biopolymères Surfaces (PBS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Centre d'élaboration de matériaux et d'études structurales (CEMES), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UPS), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Université de Bordeaux (UB), Centre National de la Recherche Scientifique (CNRS)-Institut Curie-Université Pierre et Marie Curie - Paris 6 (UPMC), Institut Curie-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), and École normale supérieure - Paris (ENS Paris)-École normale supérieure - Paris (ENS Paris)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: micropatterns, Biomedical Engineering, 02 engineering and technology, PLL-PEG antifouling, 010402 general chemistry, 01 natural sciences, redox responsive, Biomaterials, chemistry.chemical_compound, PEG ratio, Polymer chemistry, Copolymer, [CHIM]Chemical Sciences, Cell adhesion, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Chemistry, dynamic coatings, Biochemistry (medical), cell adhesion, General Chemistry, Adhesion, Polymer, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, Click chemistry, Azide, 0210 nano-technology, Ethylene glycol, disulfide
Abstract: International audience; Spontaneous adsorption of poly(lysine)-g-poly(ethyleneglycol) comb-like copolymers (PLL-g-PEG) is a versatile mean to coat substrates with polymer layers that resist cell adhesion. We prepared redox cleavable PLL-g-PEG to switch adhesion on demand. Redox sensitivity was obtained by introducing disulfide linkers between the PLL backbone and PEG strands. This modification was done alone or in combination with an azide-end on the PEG strands that enabled in situ conjugations of adhesion peptides or fluorescent labels (by simple application of commercially available molecules for copper-free click chemistry compatible with cell survival). To balance the functional (adhesion-promoting) vs cell-repellent copolymers, mixed layers of adjusted compositions were obtained by coadsorption from mixed solutions of the cleavable copolymer with non-cleavable and repellant PLL-g-PEG. The deposition of copolymers and quantitative cleavage as triggered by reductive conditions (application of solutions of tris(carboxyethyl)phosphine, dithiothreitol or gluthatione) were characterized by QCM-D, XPS, and fluorescence microscopy. In cell culture conditions, redox-triggered cleavage was obtained by non toxic application of TCEP for a few minutes, enabling either to release cell attachment points (i.e. cleavage of RGD-presenting areas) or to "open" non-specific adherent areas (i.e. transition from PEG-presenting areas to adherent PLL-like coatings).
Published: 2019

21. Effect of Zn on the grain boundary precipitates and resulting alkaline etching of recycled Al-Mg-Si-Cu alloys

Author: Linsey Lapeire, Alexander Lutz, Kim Verbeken, Luiz Henrique de Almeida, Jean Dille, Stéphane Godet, Loïc Malet, Iris De Graeve, Herman Terryn, Materials and Chemistry, Electrochemical and Surface Engineering, Materials and Surface Science & Engineering, In-Situ Electrochemistry combined with nano & micro surface Characterization, and Architectural Engineering
Subjects: Solid-state chemistry, Materials science, chemistry.chemical_element, 02 engineering and technology, Zinc, 010402 general chemistry, Precipitates, 01 natural sciences, Chimie des solides, Technologie des autres industries, Aluminium, Etching (microfabrication), Phase (matter), Materials Chemistry, Chemical composition, Preferential grain etching, TEM EDX, Anodizing, Mechanical Engineering, zinc, Metallurgy, Metals and Alloys, Métallurgie, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Aluminum (Al-Mg-Si) alloy, Etching mechanism, Mécanique sectorielle, chemistry, Mechanics of Materials, Grain boundary, 0210 nano-technology
Abstract: The Zinc level in many 6000 Al alloys (Al-Mg-Si-type) was set to a maximum of 0.03 wt% as common industrial practice. Concentrations above 0.03 wt% can modify the alkaline etching mechanism causing the surface to go from a desired smooth look associated with a grain boundary attack (GBA), into an undesired speckled appearance due to preferential grain etching (PGE), visible after anodizing. This significantly limits the ambition of reducing the carbon footprint of Aluminum by increasing the amount of recycled material in the production process. Because Cu has been reported to counteract this negative effect of Zn, the present study is dedicated to contribute to the understanding of this interaction and is focused on Zn and Cu in peak aged AlMgSi alloys. The chemical composition of the various precipitates formed in two Al6063 alloys was studied by means of TEM and EDX, whereby Zn was found in the Q phase (AlMgSiCu) grain boundary precipitates. Two alloys, with different content of Cu and Zn were studied. The Zn/Cu ratio in the bulk was similar for both alloys, but the level of Zn in the Cu containing Q particles in the grain boundaries was different. The increased Zn concentration in Q phase precipitates is believed to decrease the potential of the precipitates with respect to the surrounding matrix. Thus, the Cu/Zn ratio in these alloys is extremely important as it defines the potential differences that in turn cause either GBA or PGE., SCOPUS: ar.j, info:eu-repo/semantics/published
Published: 2019

22. Structural characterization of coevaporated Cu(In,Ga)Se2 absorbers deposited at low temperature

Author: Frédérique Donsanti, Laurent Lombez, Thibaud Hildebrandt, Valentin Achard, Daniel Lincot, Marie Jubault, Matteo Balestrieri, Jorge Posada, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Institut Photovoltaïque d’Ile-de-France (UMR) (IPVF), École polytechnique (X)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-TOTAL FINA ELF-EDF (EDF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Photovoltaïque d’Ile-de-France (ITE) (IPVF)-Air Liquide [Siège Social], Institut Photovoltaïque d’Ile-de-France (ITE) (IPVF), Institut de Recherche et Développement sur l'Energie Photovoltaïque (IRDEP), EDF R&D (EDF R&D), EDF (EDF)-EDF (EDF)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-EDF R&D (EDF R&D), and EDF (EDF)-EDF (EDF)
Subjects: Diffraction, Grazing incidence diffraction, Materials science, business.industry, Mechanical Engineering, Metals and Alloys, 02 engineering and technology, Substrate (electronics), 010402 general chemistry, 021001 nanoscience & nanotechnology, Microstructure, 01 natural sciences, Copper indium gallium selenide solar cells, 0104 chemical sciences, Mechanics of Materials, Impurity, [PHYS.COND.CM-GEN]Physics [physics]/Condensed Matter [cond-mat]/Other [cond-mat.other], Materials Chemistry, Optoelectronics, Thin film, 0210 nano-technology, business, Short circuit, ComputingMilieux_MISCELLANEOUS
Abstract: This paper focuses on low temperature (∼390 °C) growth of Cu(In,Ga)Se2 (CIGS) for high efficiency solar cells. The process developed in this work allows the growth of high quality CIGS thin films on flexible substrates such as polymer foils with lower impurity out-diffusion from the substrate. We carry out advanced analysis of the microstructure of CIGS absorbers prepared using multi-stage coevaporation on polyimide at low temperature leading to state-of-the-art efficiencies exceeding 18%. We also develop a method that can be used to easily interpret the x-ray diffraction data using compositional analysis, when asymmetric or multi-feature peaks are present. This method proves to be particularly useful to rule out in-plane inhomogeneities and undesired phases when in-depth gradients are present. This analysis is combined with electron microscopy and more advanced x-ray analysis (grazing incidence diffraction and pole plots) to create a global model of the film microstructure. We show that the film is composed of at least three stacked layers with different properties and that the microstructure of the layers has an impact on the cell performances. In particular, the short circuit current Jsc is strongly related to the intensity of the (112) peak.
Published: 2019

23. Carbon Monoxide Oxidation Promoted by a Highly Active Strained PdO Layer at the Surface of Au30Pd70(110)

Author: M.C. Saint-Lager, Francisco J. Cadete Santos Aires, O. Robach, E. Ehret, Stéphanie Garaudée, M. A. Languille, Aude Bailly, Surfaces, Interfaces et Nanostructures (SIN ), Institut Néel (NEEL), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Institut photonique d'analyse non-destructive européen des matériaux anciens (IPANEMA), Muséum national d'Histoire naturelle (MNHN)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Ministère de la Culture (MC), IRCELYON-Catalyse Hétérogène pour la Transition Energétique (CATREN), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Epitaxie et couches minces (EpiCM ), Nanostructures et Rayonnement Synchrotron (NRS ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Surfaces, Interfaces et Nanostructures (NEEL - SIN), Epitaxie et couches minces (NEEL- EpiCM), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Subjects: кислород, Materials science, Analytical chemistry, Oxide, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, Mass spectrometry, 01 natural sciences, Oxygen, Catalysis, chemistry.chemical_compound, оксид углерода, тонкие пленки, Phase (matter), каталитические свойства, золото, Dissolution, ComputingMilieux_MISCELLANEOUS, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, окисление, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 0210 nano-technology, Layer (electronics), Carbon monoxide
Abstract: International audience; The evolution of the Au30Pd70(110) surface was studied by coupling grazing incidence X-ray diffraction and mass spectrometry under oxygen-rich conditions at moderate temperatures (300 to 470 K). This allows us to correlate the depth profile of its structure to its catalytic properties for carbon monoxide (CO) oxidation. Under increasing pressure from ultrahigh vacuum up to 100 mbar, both oxygen and CO induce Pd segregation, even at room temperature. However, in pure oxygen the surface is reorganized with a (1 × 2) missing row reconstruction, whereas in pure CO it is strongly roughened. When oxygen pressure is increased a phase corresponding to the initial step of the oxidation with oxygen dissolution in the subsurface region appears at first. Then, from about 400 K onward, an oxidized thin Pd layer (≤1 nm) is formed growing in the [100]PdO direction. This PdO phase is strained and does not coincide with the P42/mmc structure usually observed for this oxide under ambient conditions. It is more probably consistent with the high pressure I4/mmm PdO structure strained by epitaxy on the underneath alloy. For higher oxidizing conditions and layer thickness, the oxide will then relax to the usual PdO structure. This strained oxide is easily reduced by CO and exhibits a very high activity for CO oxidation. Its catalytic performance at 470 K is comparable to the one found on surfaces of pure palladium at higher temperatures. Furthermore, on the clean Au30Pd70(110) surface, surface oxidation is hindered up to 470 K if CO is introduced prior to oxygen. This indicates that when Pd is alloyed with gold, its binding with CO is stronger than with oxygen. The weakening of the Pd–O binding by surrounding gold atoms is the key of the formation of a well-ordered and very active thin PdO film on Au30Pd70(110).
Published: 2019

24. Covalent and Selective Grafting of Polyethylene Glycol Brushes at the Surface of ZIF-8 for the Processing of Membranes for Pervaporation

Author: Thomas Berthelot, Elena Bellido, Florent Carn, Patricia Horcajada, Rocio Semino, Nicolas Menguy, Maria E. Dmitrenko, Guillaume Maurin, Denis Roizard, Sérgio R. Tavares, Marvin Benzaqui, Christian Serre, Nathalie Steunou, Anastasia V. Penkova, Mónica Giménez-Marqués, Anna I. Kuzminova, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Matière et Systèmes Complexes (MSC), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS), Instituto IMDEA Energía, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Service de Physique et de Chimie des Surfaces et Interfaces (SPCSI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Saint Petersburg University (SPBU), Laboratoire Réactions et Génie des Procédés (LRGP), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), ANR-10-LABX-0035,Nano-Saclay,Paris-Saclay multidisciplinary Nano-Lab(2010), European Project: 608490,EC:FP7:ENERGY,FP7-ENERGY-2013-1,M4CO2(2014), École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Matière et Systèmes Complexes (MSC (UMR_7057)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Centre National de la Recherche Scientifique (CNRS)-Université de Lorraine (UL), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Muséum national d'Histoire naturelle (MNHN)-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP UMR8004 FRE2000), École normale supérieure - Paris (ENS Paris)-École normale supérieure - Paris (ENS Paris)-ESPCI ParisTech-Centre National de la Recherche Scientifique (CNRS), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS)-Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC), Instituto IMDEA Energy, Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), and ANR: NanoSaclay,ANR-10-LABX-0035
Subjects: Vinyl alcohol, Materials science, Poly(vinyl alcohol), General Chemical Engineering, Nanoparticle, 02 engineering and technology, Polyethylene glycol, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Pervaporation, Surface modification, Dynamic light scattering, Environmental Chemistry, Membranes, Renewable Energy, Sustainability and the Environment, technology, industry, and agriculture, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, MOFs, 0104 chemical sciences, Membrane, chemistry, Chemical engineering, Membranes, MOFs, Pervaporation, Poly(vinyl alcohol), Surface modification, 0210 nano-technology, Zeolitic imidazolate framework
Abstract: International audience; The so-called Graftfast reaction in water and at room temperature (RT) was applied to graft polyethylene glycol (PEG) at the surface of the microporous zeolitic imidazolate framework ZIF-8 nanoparticles (NPs) using acrylPEG of different chain lengths (480 Da and 5 kDa). In comparison to non-modified ZIF-8 NPs, both chemical and colloidal stabilities of PEGylated ZIF-8 NPs are significantly enhanced in water. A series of colloidal complex fluids by mixing PEG grafted ZIF-8 (i. e. PEG-g-ZIF-8) NPs with different amounts of polyvinylalcohol (PVA) was prepared and characterized by advanced characterization tools such as dynamic light scattering (DLS) and small-angle X-ray scattering (SAXS) thereby showing their long-term colloidal stability. Finally, dense and supported mixed matrix membranes were cast from PEG-g-ZIF-8/PVA solutions and have shown high performance in isopropanol (IPA) dehydration by pervaporation. The permeation flux of the supported MMM (i. e. 0.091 kg/(m$^2$h) is eleven times higher than that of the pure PVA membrane and these MMMs present a high separation factor (i. e. 7326). These transport properties are presumably due to the molecular sieving effects induced by ZIF-8 and the good interfacial properties of the membrane. The computational exploration of the ZIF-8/PVA and PEG/PVA interfaces provides a microscopic scale explanation for the enhanced compatibility of PVA with the PEGylated MOF when compared to that for the composite based on the bare ZIF-8 as a filler.
Published: 2019

25. Molybdate-phosphate conversion coatings to protect steel in a simulated concrete pore solution

Author: Kitty Baert, Iris De Graeve, Hilke Verbruggen, Herman Terryn, Faculty of Engineering, Materials and Chemistry, Electrochemical and Surface Engineering, Materials and Surface Science & Engineering, In-Situ Electrochemistry combined with nano & micro surface Characterization, and Architectural Engineering
Subjects: Materials science, Chemistry(all), Phosphate, 02 engineering and technology, Molybdate, 010402 general chemistry, 01 natural sciences, Corrosion, chemistry.chemical_compound, symbols.namesake, X-ray photoelectron spectroscopy, conversion coating, Materials Chemistry, steel, Composite material, Polarization (electrochemistry), Pore solution, Surfaces and Interfaces, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Surfaces, Coatings and Films, Anode, chemistry, Conversion coating, symbols, concrete, 0210 nano-technology, Raman spectroscopy
Abstract: For the corrosion protection of steel rebars in concrete, five different molybdate-phosphate conversion coatings were prepared, by changing the molybdate-phosphate ratio in the conversion baths. Their composition and morphology were studied with GD-OES, XPS, Raman spectroscopy and SEM-EDX and a schematic representation of their structure is suggested. Further, the corrosion resistance properties of the coatings were evaluated in a simulated concrete pore solution (CPS) containing chlorides, using anodic polarization measurements. Thanks to the elaborated surface analysis their corrosion behaviour could be correlated to their structure. The results show that by altering the molybdate-phosphate ratio the structure and, consequently, the corrosion protection properties change significantly. By optimizing this ratio a twofold protection mechanism could be attained, demonstrating both good barrier properties and consistent with active corrosion protection.
Published: 2019

26. Conductivity via Thermally Induced Gap States in a Polyoxometalate Thin Layer

Author: Cindy L. Rountree, Amanda Generosi, Barbara Paci, Anna Proust, Qirong Zhu, Claire Mathieu, Nicholas Barrett, Guillaume Izzet, Pierre Gouzerh, Séverine Renaudineau, Ludovic Tortech, Xihui Liang, Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Consiglio Nazionale delle Ricerche [Roma] (CNR), Service de physique de l'état condensé (SPEC - UMR3680), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), DIM NanoK, région Ile de France, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR)
Subjects: Materials science, Photoemission spectroscopy, 02 engineering and technology, Conductivity, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Polyoxometalate Thin Layer, Physical and Theoretical Chemistry, Electrical conductor, Deposition (law), business.industry, Thermally Induced Gap- States, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Thermal conduction, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Characterization (materials science), General Energy, Polyoxometalate, Optoelectronics, 0210 nano-technology, business, Layer (electronics)
Abstract: International audience; We report a study of alpha-[P2W18O62]6-, Wells-Dawson polyoxometalate layers deposited on ITO coated glass substrates. A variety of techniques has been used including atomic force microscopy for surface topography characterization, current mapping and current-voltage characteristics, X-ray photoemission spectroscopy for chemical analysis, UV-visible photoemission spectroscopy for determination of band line-ups and energy dispersive X-ray reflectivity for determination of layer thicknesses and scattering length densities. The conditions of film deposition and subsequent thermal annealing strongly affect the film characteristics. In particular, we show that nanostriped films a few tens of nm thick can be obtained in a reproducible manner and that such structuring is accompanied by the appearance of gap-states and by a switch from an insulating to a conductive state. Current-voltage characteristics demonstrate that highly ordered films of K 6 [P 2 W 18 O 62 ] allow electron flow only from ITO to [P2W18O62]6-, thus showing a rectifying effect. Finally, we integrate the POM layer 2 into an organic photovoltaic device and show the conduction through it thanks to favorable band alignment between ITO, the gap states and the active photovoltaic layers.
Published: 2019

27. Exfoliated fluorinated carbons with a low and stable friction coefficient

Author: Marc Dubois, Elodie Petit, P. Thomas, Michael Herraiz, Nicolas Batisse, Institut de Chimie de Clermont-Ferrand (ICCF), SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Groupe de Technologie des Surfaces et Interfaces (GTSI), Université des Antilles (UA), and Groupe de Technologie des Surfaces et Interfaces [URp2_2] (GTSI)
Subjects: Materials science, Carbon nanofiber, General Chemical Engineering, chemistry.chemical_element, 02 engineering and technology, General Chemistry, Tribology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Exfoliation joint, 0104 chemical sciences, Chemical engineering, chemistry, Nanofiber, [CHIM]Chemical Sciences, Atomic ratio, Graphite, 0210 nano-technology, Carbon, Dry lubricant
Abstract: International audience; Exfoliation appears as a promising way to decrease the friction coefficient of carbon materials. Although there is massive defluorination during exfoliation, the friction coefficient is not increased and an exfoliated structure facilitates the formation of a homogeneous and stable tribofilm. The weakening of the interparticle interactions due to the exfoliation process is the main explanation for the excellent tribological properties. Three representative examples are studied to evidence the efficiency of the thermal shock to prepare solid lubricants or additives for lubricating oils, high temperature graphite fluorides, fluorinated carbon nanofibers and fluorinated nanodiscs. An opened (graphite fluoride) or defect structure (nanofibers) allows the gases formed during the exfoliation to be evolved; the exfoliation is then successful regardless of the C–F bonding. Exfoliation and defluorination occur simultaneously resulting in samples with a low F/C atomic ratio. On the contrary for the case of fluorinated nanodiscs, the exfoliation fails because of cracks and edges as well as the low diameter of the discs.
Published: 2019

28. Dual-action self-healing protective coatings with photothermal responsive corrosion inhibitor nanocontainers

Author: Jinke Wang, Lingwei Ma, Panjun Wang, Dawei Zhang, Yao Huang, Herman Terryn, Hongchang Qian, Luyao Huang, Johannes M. C. Mol, Xiaogang Li, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: corrosion inhibitor, Materials science, Chemistry(all), General Chemical Engineering, Nanoparticle, Nanotechnology, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, Industrial and Manufacturing Engineering, Corrosion, Corrosion inhibitor, chemistry.chemical_compound, shape memory polymer, Coating, Environmental Chemistry, Plasmonic titanium nitride, Benzotriazole, Photothermal response, General Chemistry, Epoxy, Photothermal therapy, 021001 nanoscience & nanotechnology, Titanium nitride, 0104 chemical sciences, self-healing coating, chemistry, visual_art, engineering, visual_art.visual_art_medium, Chemical Engineering(all), 0210 nano-technology
Abstract: This work introduces a novel nanocomposite coating with dual-action self-healing corrosion protection activated by the photothermal response of plasmonic titanium nitride nanoparticles (TiN NPs). TiN@mesoporous SiO2 core–shell nanocontainers were developed as reservoirs for benzotriazole (BTA) corrosion inhibitors and incorporated into the shape memory epoxy coating matrix. Under near-infrared (NIR) light irradiation, the thermogenesis effect of TiN could not only promote the release of corrosion inhibitors from nanocontainers into the crevice, but also trigger the shape memory effect of damaged epoxy to merge the coating scratch. As such, the dual-action self-healing mechanisms combining the formation of an inhibitor-based protective layer and the scratch closure efficiently suppressed the corrosion process at the exposed metal surface. Surface characterization and electrochemical measurement results proved that the nanocomposite coating incorporated with 2 wt% of TiN-BTA@SiO2 exhibited the optimal corrosion protection as well as an excellent self-healing performance that can be initiated within 30 s of NIR illumination. This photo-controlled self-healing approach is potentially useful in designing next-generation self-healing coatings with ultrafast response time and high healing efficiency.
Published: 2021

29. Dimensional measurement of TiO$_2$ (Nano) particles by SAXS and SEM in powder form

Author: Najoua Bouzakher-Ghomrasni, Jocelyne Leroy, Fabienne Testard, Olivier Taché, Carine Chivas-Joly, Nicolas Feltin, Laboratoire National de Métrologie et d'Essais [Trappes] (LNE ), Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), With the financial support from Agence Nationale Recherche Technologie (ANRT)under the contract CIFRE N°2018/0367., Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685)
Subjects: Small-angle X-ray scattering, Chemistry, 010401 analytical chemistry, Nanoparticle, 02 engineering and technology, SAXS, [CHIM.MATE]Chemical Sciences/Material chemistry, Raw material, 021001 nanoscience & nanotechnology, Metrology, 01 natural sciences, 0104 chemical sciences, Analytical Chemistry, Characterization (materials science), (Nano)particles, Manufactured products, Specific surface area, Nano, SEM, TiO2, Manufactured nanoparticles, Composite material, 0210 nano-technology
Abstract: International audience; The market for nano-additive materials has been growing exponentially since 2012, with almost 5040 consumer products containing nanoparticles in 2021. In parallel, the increasing recommendations, definitions and legislations underline the need for traceability of manufactured nanoparticles and for methods able to identify and quantify the “nano” dimensional character in manufactured product. From a multi-technic approach, this paper aims to compare the mesurands extracted from SAX/BET (specific surface area) and SEM (diameter equivalent to a projected surface area) on different TiO$_2$ powder issued from referenced, synthesized materials, raw materials (additives) and extracted materials from manufactured products. The influence of various parameters such as the anisotropic factor, the interaction between particles, the size distribution and the extraction steps are discussed to illustrate their impact on the diameter values issued from two different measurands. These results illustrate the difficulties in (nano)particles characterization. SEM and SAXS are complementary technics depending on the level of dimensional characterization required.
Published: 2021

30. Solution-processed graphene–nanographene van der Waals heterostructures for photodetectors with efficient and ultralong charge separation

Author: Loïc Rondin, Artur Ciesielski, Paolo Samorì, Gvido Bratina, Mischa Bonn, Shuai Fu, Hai I. Wang, Zhaoyang Liu, Shen Zhao, Xuelin Yao, Alex G. Dixon, Haixin Qiu, Egon Pavlica, Can Wang, Akimitsu Narita, Klaus Müllen, Jean-Sébastien Lauret, Stéphane Campidelli, Palacin, Serge, Center of Chemistry of Complex System - - CSC2010 - ANR-10-LABX-0026 - LABX - VALID, Boites quantiques et Nanorubans de Graphene pour l'optique - - GRANAO2019 - ANR-19-CE09-0031 - AAPG2019 - VALID, Supramolecular engineering of multifunctional systems and devices: the molecular approach to 2D materials - SUPRA2DMAT - 833707 - INCOMING, Graphene Flagship Core Project 3 - GrapheneCore3 - - H20202020-04-01 - 2023-09-30 - 881603 - VALID, Institut de Science et d'ingénierie supramoléculaires (ISIS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Max Planck Institute for Polymer Research, Max-Planck-Gesellschaft, Laboratory of Organic Matter Physics, University of Nova Gorica, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Carbon Nanomaterials Unit, Okinawa Institute of Science and Technology Graduate University (OIST), the German Research Foundation (DFGProjektnummer 182087777-SFB 951), the Slovenian Research Agency (research core funding No. P1-0055), ANR-10-LABX-0026,CSC,Center of Chemistry of Complex System(2010), ANR-19-CE09-0031,GRANAO,Boites quantiques et Nanorubans de Graphene pour l'optique(2019), European Project: 833707,SUPRA2DMAT, European Project: 881603,H2020,H2020-SGA-FET-GRAPHENE-2019, GrapheneCore3(2020), Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), and Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685)
Subjects: Nanostructure, Terahertz radiation, Photodetector, 02 engineering and technology, Specific detectivity, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Biochemistry, Catalysis, law.invention, Responsivity, Colloid and Surface Chemistry, Physisorption, law, [CHIM.MATE] Chemical Sciences/Material chemistry, business.industry, Graphene, Chemistry, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Exfoliation joint, 0104 chemical sciences, Optoelectronics, 0210 nano-technology, business
Abstract: International audience; Sensitization of graphene with inorganic semiconducting nanostructures has been demonstrated as a powerful strategy to boost its optoelectronic performance. However, the limited tunability of optical properties and toxicity of metal cations in the inorganic sensitizers prohibits their widespread applications, and the in-depth understanding of the essential interfacial charge-transfer process within such hybrid systems remains elusive. Here, we design and develop high-quality nanographene (NG) dispersions with a large-scale production using high-shear mixing exfoliation. The physisorption of these NG molecules onto graphene gives rise to the formation of graphene–NG van der Waals heterostructures (VDWHs), characterized by strong interlayer coupling through $\pi$–$\pi$ interactions. As a proof of concept, photodetectors fabricated on the basis of such VDWHs show ultrahigh responsivity up to 4.5 × 10$^7$ A/W and a specific detectivity reaching 4.6 × 10$^{13}$ Jones, being competitive with the highest values obtained for graphene-based photodetectors. The outstanding device characteristics are attributed to the efficient transfer of photogenerated holes from NGs to graphene and the long-lived charge separation at graphene–NG interfaces (beyond 1 ns), as elucidated by ultrafast terahertz (THz) spectroscopy. These results demonstrate the great potential of such graphene–NG VDWHs as prototypical building blocks for high-performance, low-toxicity optoelectronics.
Published: 2021

31. Laser induced breakdown spectroscopy for plastic analysis

Author: Jong-Min Lee, Jean-Christophe P. Gabriel, Qiang Zeng, Chor Yong Tay, Jean-Baptiste Sirven, School of Chemical and Biomedical Engineering, School of Materials Science and Engineering, Energy Research Institute @ NTU (ERI@N), Energy Research Institute, Nanyang Technological University [Singapour], School of Chemical & Biomedical Engineering, Service d'études analytiques et de réactivité des surfaces (SEARS), Département de Physico-Chimie (DPC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), School of Materials Science and Engineering [Singapore], SCARCE, which is supported by the National Research Foundation, Prime Minister’s Office, Singapore, the Ministry of National Development, Singapore, and National Environment Agency, Ministry of Sustainability and the Environment, Singapore under the Closing the Waste Loop R&D Initiative as part of the Urban Solutions & Sustainability – Integration Fund (Award No. USS-IF-2018-4), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Plastic recycling, Materials science, Materials [Engineering], business.industry, 010401 analytical chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 01 natural sciences, 0104 chemical sciences, Analytical Chemistry, Laser induced breakdown spectroscopy (LIBS), Online analysis, Chemistry [Science], Laser-induced breakdown spectroscopy, Process engineering, business, Qualitative, Spectroscopy, Analysis method, Plastic Recycling, Quantitative
Abstract: The huge consumption of modern plastic with improper disposals has posed a great threat to the environment and human beings. To put these post-consumer plastics into the recycling chain, laser induced breakdown spectroscopy (LIBS) has been established as a potential tool for rapid grading of plastics online. Meanwhile, LIBS is a powerful tool for plastic investigations in the laboratory with the capacity of simultaneous qualitative and quantitative analysis. The present review describes the development and prospect of plastic investigations using LIBS, highlighting the intrinsic advantages of LIBS for plastic recycling. Moreover, the selection of hardware components and analysis methods are discussed, which may help to start a research on plastic using LIBS. National Environmental Agency (NEA) National Research Foundation (NRF) The authors are grateful for the financial support from SCARCE, which is supported by the National Research Foundationgs2:, Prime Minister's Office, Singapore, the Ministry of National Development, Singapore, and National Environment Agency, Ministry of Sustainability and the Environment, Singapore under the Closing the Waste Loop R&D Initiative as part of the Urban Solutions & Sustainability - Integration Fund (Award No. USS-IF-2018-4).
Published: 2021

32. From NiMoO 4 to γ-NiOOH: Detecting the Active Catalyst Phase by Time Resolved in Situ and Operando Raman Spectroscopy

Author: Pierfrancesco Maltoni, Robin N. Dürr, Bruno Jousselme, Haining Tian, Leif Hammarström, Tomas Edvinsson, Uppsala University, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Departement of engineering sciences, the Angstrom Laboratory, the Swedish Research Council (VR) Grant 2015-03814, European Project: 765376,eSCALED, Department of Chemistry – Ångström Laboratory, UPPSALA University, Box 538, 75120, Uppsala, Sweden, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: Materials science, General Physics and Astronomy, chemistry.chemical_element, Materialkemi, 02 engineering and technology, engineering.material, nickel molybdate, 010402 general chemistry, Electrocatalyst, 01 natural sciences, 7. Clean energy, Physical Chemistry, Article, Catalysis, time-resolved operando Raman spectroscopy, symbols.namesake, Phase (matter), nanostructures, Materials Chemistry, electrocatalysis, General Materials Science, molybdenum leaching, Fysikalisk kemi, General Engineering, Oxygen evolution, in situ catalyst formation, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, chemistry, 13. Climate action, Molybdenum, symbols, engineering, alkaline water splitting, Noble metal, Nanorod, Additions and Corrections, 0210 nano-technology, Raman spectroscopy
Abstract: Water electrolysis powered by renewable energies is a promising technology to produce sustainable fossil free fuels. The development and evaluation of effective catalysts are here imperative; however, due to the inclusion of elements with different redox properties and reactivity, these materials undergo dynamical changes and phase transformations during the reaction conditions. NiMoO4 is currently investigated among other metal oxides as a promising noble metal free catalyst for the oxygen evolution reaction. Here we show that at applied bias, NiMoO4·H2O transforms into γ-NiOOH. Time resolved operando Raman spectroscopy is utilized to follow the potential dependent phase transformation and is collaborated with elemental analysis of the electrolyte, confirming that molybdenum leaches out from the as-synthesized NiMoO4·H2O. Molybdenum leaching increases the surface coverage of exposed nickel sites, and this in combination with the formation of γ-NiOOH enlarges the amount of active sites of the catalyst, leading to high current densities. Additionally, we discovered different NiMoO4 nanostructures, nanoflowers, and nanorods, for which the relative ratio can be influenced by the heating ramp during the synthesis. With selective molybdenum etching we were able to assign the varying X-ray diffraction (XRD) pattern as well as Raman vibrations unambiguously to the two nanostructures, which were revealed to exhibit different stabilities in alkaline media by time-resolved in situ and operando Raman spectroscopy. We advocate that a similar approach can beneficially be applied to many other catalysts, unveiling their structural integrity, characterize the dynamic surface reformulation, and resolve any ambiguities in interpretations of the active catalyst phase. Addition/correction: This article has been corrected. Correction in: ACS Nano 2021, 15, 12, 20693-20693. DOI: 10.1021/acsnano.1c10145Title in Web of Science: From NiMoO4 to gamma-NiOOH: Detecting the Active Catalyst Phase by Time Resolved in Situ and Operando Raman Spectroscopy
Published: 2021

33. Ion yield enhancement at the organic/inorganic interface in SIMS analysis using Ar-GCIB

Author: Claude Poleunis, Priya Laha, Pierre Eloy, Arnaud Delcorte, Vanina Cristaudo, Herman Terryn, Tom Hauffman, UCL - SST/IMCN/BSMA - Bio and soft matter, Materials and Chemistry, Electrochemical and Surface Engineering, and Materials and Surface Science & Engineering
Subjects: Ion signal enhancement factor, Materials science, Silicon, Chemistry(all), Analytical chemistry, General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, polystyrene, Physics and Astronomy(all), 010402 general chemistry, 01 natural sciences, Ion, Irganox 1010, Sputtering, Fragmentation, Ionization, fragmentation, Wafer, Polystyrene, chemistry.chemical_classification, Argon, General Chemistry, Polymer, Surfaces and Interfaces, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Irganox1010, 0104 chemical sciences, Surfaces, Coatings and Films, Secondary ion mass spectrometry, chemistry, Sputtering yield volume, 0210 nano-technology, ToF-SIMS
Abstract: Argon gas cluster ion beams (Ar-GCIBs) provide new opportunities for molecular depth profiling and imaging of organic materials and biological samples, thanks to recent technological developments that have led to the construction of new SIMS spectrometers where the traditional issues related to their low lateral resolution along with poor mass resolution and mass accuracy are overcome. The present fundamental contribution on SIMS molecular depth profiling investigates the variations of the secondary ion signals observed at the organic–inorganic hybrid interface when using Ar-GCIB as the analytical beam. With this in mind, depth profiling experiments were performed with a ToF-SIMS spectrometer using different analysis beams: 30-keV Bi5+ versus 10-keV Arn+ with a cluster size (n) of 800, 1500, 3000 and 5000 atoms, respectively. A 10-keV Ar3000+ beam was used for sputtering in all the experiments. Irganox 1010 and model polymers such as polystyrene (PS) and poly (methyl methacrylate) (PMMA) oligomers were chosen. Silicon wafer and a polymer-based substrates were employed to test materials with different stiffness, which is directly related to their Young’s moduli, an important parameter in this study. Ar-GCIB depth profiles systematically show ion signal enhancement of the characteristic fragments of PS and Irganox 1010 when approaching the interface with the silicon substrate, that can reach up to 60% for [M1010-H]− in Irganox films deposited onto silicon wafers. This enhancement increases with increasing n in both ion polarities. These results point out some ionization effects on the observed signal enhancement at the interface. The experimental observations will be explained on the basis of the physics of the impact of large argon clusters on different target materials and the energy confinement of the ion projectile in the organic overlayers. Finally, the thickness of organic films on rigid substrates in the nanoscale appears to be a crucial parameter to dramatically improve the sensitivity to molecular fragments when using large Ar cluster ions as analysis beams.
Published: 2021

34. Fine tuning the structural colours of photonic nanosheet suspensions by polymer doping

Author: Laurent J. Michot, Henricus H. Wensink, Jean-Christophe P. Gabriel, Patrick Davidson, Karin El Rifaii, Claire Goldmann, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), CEA: Programme Transversal Nanosciences, ANR-17-CE04-0003,4WATER,Pour la Surveillance de la qualité de l'eau(2017), European Project: 320915,EC:FP7:ERC,ERC-2012-ADG_20120216,REE-CYCLE(2013), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: chemistry.chemical_classification, [PHYS]Physics [physics], Phase transition, Aqueous solution, Materials science, 02 engineering and technology, General Chemistry, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Membrane, chemistry, Chemical engineering, Phase (matter), DLVO theory, [CHIM]Chemical Sciences, Lamellar structure, 0210 nano-technology, [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], Nanosheet
Abstract: International audience; Aqueous suspensions of nanosheets are readily obtained by exfoliating low-dimensional mineral compounds like H3Sb3P2O14. The nanosheets self-organize, at low concentration, into a periodic stack of membranes, i.e. a lamellar liquid-crystalline phase. Due to the dilution, this stack has a large period of a few hundred nanometres, it behaves as a 1-dimensional photonic material and displays structural colours. We experimentally investigated the dependence of the period on the nanosheet concentration. We theoretically showed that it cannot be explained by the usual DLVO interaction between uniform lamellae but that the particulate nature of nanosheet-laden membranes must be considered. Moreover, we observed that adding small amounts of 100 kDa poly(ethylene oxide) (PEO) decreases the period and allows tuning the colour throughout the visible range. PEO adsorbs on the nanosheets, inducing a strong reduction of the nanosheet charge. This is probably due to the Lewis-base character of the EO units of PEO that become protonated at the low pH of the system, an interpretation supported by theoretical modeling. Oddly enough, adding small amounts of 1 MDa PEO has the opposite effect of increasing the period, suggesting the presence of an additional intermembrane repulsion not yet identified. From an applied perspective, our work shows how the colours of these 1-dimensional photonic materials can easily be tuned not only by varying the nanosheet concentration (which might entail a phase transition) but also by adding PEO. From a theoretical perspective, our approach represents a necessary step towards establishing the phase diagram of aqueous suspensions of charged nanosheets.
Published: 2021

35. Nanostructured intermetallic InSb as a high-capacity and high-performance negative electrode for sodium-ion batteries

Author: Jocelyne Leroy, Magali Gauthier, Eddy Foy, Irshad Mohammad, Eric Leroy, Lucie Blondeau, Hicham Khodja, Laboratoire d'Etudes des Eléments Légers (LEEL - UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Archéomatériaux et Prévision de l'Altération (LAPA - UMR 3685), Institut de Recherches sur les Archéomatériaux (IRAMAT), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Université Bordeaux Montaigne-Université de Technologie de Belfort-Montbeliard (UTBM), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Institut de Chimie et des Matériaux Paris-Est (ICMPE), Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), ANR-16-CE05-0004,MAGICIEN,MAGnésium-Ion: batteries haute Capacité Innovantes à base d'Electrodes négatives Nanostructurées(2016), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Technologie de Belfort-Montbeliard (UTBM)-Université d'Orléans (UO)-Université Bordeaux Montaigne (UBM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), and Université de Technologie de Belfort-Montbeliard (UTBM)-Université d'Orléans (UO)-Université Bordeaux Montaigne-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Renewable Energy, Sustainability and the Environment, Sodium, Intermetallic, Energy Engineering and Power Technology, chemistry.chemical_element, 02 engineering and technology, Electrolyte, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 0104 chemical sciences, Dielectric spectroscopy, Fuel Technology, X-ray photoelectron spectroscopy, Chemical engineering, chemistry, Electrode, Coupling (piping), 0210 nano-technology
Abstract: International audience; Following the trends of alloys as negative electrodes for Na-ion batteries, the sodiation of the InSb intermetallic compound was investigated for the first time. The benefit of coupling Sb with In was evaluated through the synthesis of InSb by a chemical reduction in the form of nanostructured particles assembled in micrometric aggregates. After a full structural, morphological and surface characterization, the electrochemical performance of nanostructured InSb was examined in a carbonated electrolyte with fluoroethylene carbonate (FEC) as additive. The performance turns out to be remarkable with a capacity around 450 mAh g-1 after 50 cycles at C/5. In terms of cyclability, the capacity of InSb is impressively stable at 1C with a capacity retention of 96 % up to 100 cycles, in contrast to the strong capacity decay observed for a nanostructured Sb powder produced in a similar fashion. A good high-rate behavior is also observed with a capacity of 310 mAh g-1 at 5C. The better stability of the InSb compound compared to pure Sb suggests that combining In with Sb improves the ability of the material to alleviate volume expansion and mechanical stress during the repeated sodiation/desodiation processes. Surface and structural characterization by X-Ray photoelectron spectroscopy, X-Ray diffraction and electrochemical impedance spectroscopy after cycling were finally implemented to shed light on the SEI composition and electrochemical behavior of the promising InSb compound.
Published: 2021
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36. Electrocatalytic hydrogen evolution reaction promoted by Co/N/C catalysts with Co−N x active sites derived from precursors forming N-doped graphene Nanoribbons

Author: Takashi Hayashi, Koki Matsumoto, Stéphane Campidell, Onoda Akira, Faculty of Environmental Earth Science [Sapporo], Hokkaido University [Sapporo, Japan], Division of Applied Chemistry, Graduate School of Engineering, Osaka University, Osaka University [Osaka], Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Chemistry, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, Hydrogen evolution reaction, 0104 chemical sciences, Catalysis, Nitrogen-doped graphene nanoribbon, Co/N/C catalyst, Hydrogen evolution, Doped graphene, 0210 nano-technology
Abstract: International audience; Cobalt and nitrogen co-doped carbon (Co/N/C) catalysts prepared by pyrolysis are promising electrocatalysts for hydrogen evolution reaction (HER). Construction of Co−N$_x$ active sites is an important strategy for improving HER activity. We developed a method for thermally controlled construction of the Co−N$_x$ active sites by applying a bottom-up synthetic methodology using an N-doped graphene nanoribbon (N-GNR). Preorganized aromatic rings in the precursors assist graphitization during generation of N-GNR which has N2 sites that coordinate to a cobalt ion. Atomically dispersed Co−N$_x$ sites in the catalysts are observed by electron microscopy. Moreover, the amount of Co−N$_x$ sites increases up to 0.31 wt% as confirmed by XPS and elemental analysis. The Co/N/C catalyst prepared from the precisely designed precursor forming an N-GNR shows HER activity with a low overpotential of 258 mV (in 1.0 M HClO$_{4aq}$) and 311 mV (in 0.1 M HClO$_{4aq}$) at 10 mA·cm$^{−2}$, and with a long-term stability.
Published: 2021

37. Electrochemical and surface characterization study on the corrosion inhibition of mild steel 1030 by the cationic surfactant cetrimonium trans-4-hydroxy-cinnamate

Author: Herman Terryn, Mahdi Ghorbani, Laura L. Machuca, Maria Forsyth, Jhonatan Soto Puelles, Ruhamah Yunis, Anthony Somers, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: chemistry.chemical_classification, Chemistry(all), General Chemical Engineering, Cationic polymerization, Salt (chemistry), 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, Article, 0104 chemical sciences, Corrosion, Chemistry, chemistry, Pulmonary surfactant, Chemical Engineering(all), 0210 nano-technology, QD1-999, Nuclear chemistry
Abstract: Effective corrosion inhibition of mild steel 1030 at 0.01 M NaCl concentration was achieved by the use of the nontoxic surfactant salt cetrimonium trans-4-hydroxy-cinnamate (CTA-4OHcinn). Polarization analysis on the steel samples immersed for 24 h in the control and CTA- 4OHcinn-containing solutions shows the development of a passivation potential that is more obvious at higher inhibitor concentrations along with a maximum inhibition efficiency of 97.8%. Electrochemical impedance spectroscopy (EIS) pinpoints the effect of the inhibitor on the corroding regions of the metal surface, showing an increase in the local electric resistance and conversely a decrease in the local capacitance, which indicates that the charge transfer in the corroding regions is being hindered by a deposition process. This is consistent with scanning electron microscopy (SEM) images, showing the presence of a porous oxide matrix that fills localized corrosion sites on the metal surface after 24 h of immersion in a 0.01 M NaCl + 10 mM inhibitor solution. Additionally, SEM analysis also shows the formation of an organic film surrounding the defects that is able to shield chloride attack. As a result of diffusion of chloride from the defects below the protective film, filiform corrosion can be seen. Time-resolved impedance analysis over the first 120 min of immersion in the control and inhibitor solution shows that significant inhibitor protection does not take place immediately and there is a lag phase in the first 50 min of immersion, suggesting that early localized corrosion drives further adsorption of inhibitor micelles on the metal surface. This is in agreement with X-ray photoelectron spectroscopy (XPS) analysis, which indicates a complete surface coverage over the first 2 h of immersion in a concentrated inhibitor solution. XPS also shows the heterogeneity of the film, where some parts are poorly covered, revealing the underlying surface containing iron.
Published: 2021

38. Thermally Controlled Construction of Fe–N x Active Sites on the Edge of a Graphene Nanoribbon for an Electrocatalytic Oxygen Reduction Reaction

Author: Takashi Hayashi, Akira Onoda, Tomoyuki Kitano, Hidehiro Yasuda, Koki Matsumoto, Takao Sakata, Stéphane Campidelli, Division of Applied Chemistry, Graduate School of Engineering, Osaka University, Osaka University [Osaka], Faculty of Environmental Earth Science [Sapporo], Hokkaido University [Sapporo, Japan], Analysis Technology Center, Nippon Shokubai Co., Ltd, Research Center for Ultra-High Voltage Electron Microscopy, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), JSPS KAKENHI Grant Numbers JP25708031, JP15H03857, JP15H05804, and JP19K22202, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: Materials science, Graphene, chemistry.chemical_element, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Catalysis, X-ray absorption fine structure, law.invention, Metal, X-ray photoelectron spectroscopy, chemistry, Chemical engineering, law, visual_art, visual_art.visual_art_medium, Reversible hydrogen electrode, General Materials Science, 0210 nano-technology, Carbon, Pyrolysis
Abstract: International audience; Pyrolytically prepared iron and nitrogen codoped carbon (Fe/N/C) catalysts are promising nonprecious metal electrocatalysts for the oxygen reduction reaction (ORR) in fuel cell applications. Fabrication of the Fe/N/C catalysts with Fe–Nx active sites having precise structures is now required. We developed a strategy for thermally controlled construction of the Fe–Nx structure in Fe/N/C catalysts by applying a bottom-up synthetic methodology based on a N-doped graphene nanoribbon (N-GNR). The preorganized aromatic rings within the precursors assist graphitization during generation of the N-GNR structure with iron-coordinating sites. The Fe/N/C catalyst prepared from the N-GNR precursor, iron ion, and the carbon support Vulcan XC-72R provides a high onset potential of 0.88 V (vs reversible hydrogen electrode (RHE)) and promotes efficient four-electron ORR. X-ray absorption fine structure (XAFS) and X-ray photoelectron spectroscopy (XPS) studies reveal that the N-GNR precursor induces the formation of iron-coordinating nitrogen species during pyrolysis. The details of the graphitization process of the precursor were further investigated by analyzing the precursors pyrolyzed at various temperatures using MgO particles as a sacrificial template, with the results indicating that the graphitized structure was obtained at 700 °C. The preorganized N-GNR precursors and its pyrolysis conditions for graphitization are found to be important factors for generation of the Fe–Nx active sites along with the N-GNR structure in high-performance Fe/N/C catalysts for the ORR.
Published: 2021

39. Destabilization of the Nematic Phase of Clay Nanosheet Suspensions by Polymer Adsorption

Author: Karin El Rifaii, Laurent J. Michot, Jean-Christophe P. Gabriel, Patrick Davidson, Thomas Bizien, Henricus H. Wensink, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Beamline SWING, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), ANR-17-CE04-0003,4WATER,Pour la Surveillance de la qualité de l'eau(2017), Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, polymer, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Rheology, Liquid crystal, Phase (matter), Electrochemistry, General Materials Science, beidellite, ComputingMilieux_MISCELLANEOUS, Spectroscopy, polyethylene oxide, liquid-crystal, Phase diagram, Nanosheet, [PHYS]Physics [physics], chemistry.chemical_classification, Surfaces and Interfaces, Polymer adsorption, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, adsorption, dextran, Clay, 0210 nano-technology, nematic
Abstract: International audience; Complex aqueous mixtures comprised of swelling clays and hydrosoluble polymers naturally occur in soils and play a major role in pedogenesis. They are also very often used for formulating oil-well drilling fluids, paints, and personal-care products. The suspensions of some natural clays, thanks to their large nanoparticle aspect ratio, spontaneously form nematic liquid-crystalline phases where the particles align parallel to each other, which affects their flow properties. We observed that adding small amounts of hydrosoluble polymers to these clay suspensions destabilizes the nematic phase with respect to the isotropic (disordered) phase. The polymers that we used (poly(ethylene oxide) and dextran) were too small to adopt particle-bridging conformations and small-angle X-ray scattering experiments showed that the structure of the nematic phase is not altered by polymer doping. However, the adsorption isotherm shows that the macromolecules adsorb onto the clay nanosheets, effectively coating them with a polymer layer. Our extension of Onsager’s theory for polymer-coated platelets properly captures the experimental phase diagram and shows how the nematic phase destabilization can be due to the polymer adsorbing more on the platelet faces than at the rim. Because the flow properties of the nematic phase are very different from those of the isotropic phase, the presence or absence of the former phase is an important factor to be determined and considered to explain the rheological behavior of these complex systems.
Published: 2020

40. Time Resolved Photoemission to Unveil Electronic Coupling Between Absorbing and Transport Layers in a Quantum Dot Based Solar Cell

Author: Nadine Witkowski, Adrien Khalili, Charlie Gréboval, Corentin Dabard, Julien Ramade, Prachi Rastogi, Junling Qu, Hervé Cruguel, Emmanuel Lhuillier, Audrey Chu, Tung Huu Dang, Abdelkarim Ouerghi, Mathieu G. Silly, Physico-chimie et dynamique des surfaces (INSP-E6), Institut des Nanosciences de Paris (INSP), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et d'Etude des Matériaux (UMR 8213) (LPEM), Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), ANR-18-CE30-0023,IPER-Nano2,Nanocristaux de perovskite inorganique pour la nanophotonique(2018), ANR-19-CE09-0017,FRONTAL,Nanocristaux Colloïdaux Dopés Infrarouges(2019), ANR-19-CE24-0022,COPIN,Détecteur plasmonique à nanoCristaux colloïdaux: une nouvelle filière pour l'OPtoélectronique INfrarouge(2019), ANR-19-CE09-0026,GRaSkop,Tuning Giant Rashba Spin-Orbit Coupling in Polar Single Layer Transition Metal Dichalcogenides(2019), ANR-10-LABX-0067,MATISSE,MATerials, InterfaceS, Surfaces, Environment(2010), and European Project: 756225,blackQD
Subjects: Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, law.invention, Colloid, chemistry.chemical_compound, law, Solar cell, Lead sulfide, Physical and Theoretical Chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Photodiode, Coupling (electronics), General Energy, chemistry, Quantum dot, Optoelectronics, 0210 nano-technology, business
Abstract: International audience; Lead sulfide (PbS) colloidal quantum dots-based photodiodes are remarkable structures obtained via colloidal engineering because of their outstanding optoelectronic performances. They combine surface ligand engineering to design a p-n junction with all solution processability. Here we investigate the PbS diode electronic structure combining static and dynamic photoemissions with transport measurements. We show that the n-type nature of the I-capped PbS CQDs shifts the valence band away from the Fermi level compared to the thiol capped nanocrystals. This change in majority carriers can be probed using time resolved X-ray photoemission spectroscopy (TRXPS). We also prove that the photo-induced binding energy shift depends on the nanoparticle surface chemistry. Finally, we demonstrate the ability of TRXPS to selectively probe the electronic structure of each side of an interface. We explore the PbS/MoO3 interface used as hole extractor in the PbS solar cell, using this method. We demonstrate that the PbS layer photosensitizes the MoO3 layer and that the two layers have a quasi-rigid electrostatic coupling. We identify the band bending occurring on the PbS(EDT)/MoO3 to be a limiting factor for the device performance and suggest strategies to overcome this limitation.
Published: 2020

41. Characterizing surface states in hematite nanorod photoanodes, both beneficial and detrimental to solar water splitting efficiency

Author: Dris Ihiawakrim, Adam P. Hitchcock, Stefan Stanescu, D. Stanescu, Victoria Villard, S. G. Chiuzbaian, Jocelyne Leroy, Cristian Mocuta, Mekan Piriyev, Adrien Besson, Ovidiu Ersen, Laboratoire Nano-Magnétisme et Oxydes (LNO), Service de physique de l'état condensé (SPEC - UMR3680), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), McMaster University Hamilton - Department of Chemistry & Chemical Biology, Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique
Subjects: Diffraction, Nanostructure, Materials science, Renewable Energy, Sustainability and the Environment, 02 engineering and technology, General Chemistry, Electronic structure, [CHIM.MATE]Chemical Sciences/Material chemistry, Hematite, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, X-ray photoelectron spectroscopy, Chemical engineering, visual_art, Microscopy, visual_art.visual_art_medium, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Materials Science, Nanorod, 0210 nano-technology, Surface states
Abstract: International audience; The perfomance of hematite and Ti-substituted hematite nanorods as photoanodes for solar water splitting was quantitavely evaluated from photoelectrochemical point of view. The nanostructure, morphology and chemical / electronic structure were characterized using various complementary methods, including X-ray diffraction, electron microscopy, X-ray photoelectron spectroscopy and scanning transmission X-ray microscopy. The presence of both reductive and oxidative surface states was evidenced and their impact on the photoelectrochemical efficiency was characterized. We show that both electronic conduction enhancement provided by the Ti substitution and charge transfer promoted by oxidative surface states improve solar water splitting performance.
Published: 2020

42. Water Permeation in coatings

Author: Herman Terryn, G. Van Assche, Ehsan Jalilian, Faculty of Engineering, Materials and Chemistry, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Physical Chemistry and Polymer Science
Subjects: Isothermal microcalorimetry, Thermogravimetric analysis, Materials science, characterization methods, Analytical chemistry, Infrared spectroscopy, Sorption, methodology, 02 engineering and technology, Surfaces and Interfaces, General Chemistry, coatings, Permeation, 010402 general chemistry, 021001 nanoscience & nanotechnology, Thermal diffusivity, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Corrosion, Colloid and Surface Chemistry, Solubility, 0210 nano-technology
Abstract: The objective of this work is to develop and evaluate experimental approaches with different analytical techniques to measure the permeability, diffusivity, and solubility of water in model coatings. These properties are of primary relevance in studies of coatings for corrosion protection. For water permeation measurements, setups were designed and prepared to facilitate measurements by microcalorimetry, gravimetry, and thermogravimetric analysis. For sorption measurements, films were prepared in various thicknesses to allow a proper analysis with Fourier-transform infrared spectroscopy in transmission mode and gravimetry. Both methods are successful in following water uptake kinetic curves, being complementary in film thickness ranges that can be analyzed. The validity of the permeabilities calculated from permeation measurements is compared to results from group contribution methods and reported values in the literature. Diffusivities were determined using data from the transient region in sorption and permeation measurements, as well as from the steady-state permeation rate and equilibrium solubility in permeation and sorption measurements, respectively.
Published: 2020

43. The role of hydrogen bond donor and water content on the electrochemical reduction of Ni2+ from solvents - an experimental and modelling study

Author: Andrea Ceglia, Joost De Strycker, Monika Lukaczynska-Anderson, Krista Van den Bergh, Herman Terryn, Mesfin Haile Mamme, Frank De Proft, Jon Ustarroz, Materials and Chemistry, Brussels Photonics Team, Chemistry, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Faculty of Engineering
Subjects: Hydrogen bond, General Physics and Astronomy, chemistry.chemical_element, Chimie des surfaces et des interfaces, 02 engineering and technology, Electrolyte, Chronoamperometry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 0104 chemical sciences, Catalysis, Metal, Nickel, chemistry, Chemical engineering, visual_art, visual_art.visual_art_medium, Physical and Theoretical Chemistry, Cyclic voltammetry, 0210 nano-technology
Abstract: Deep Eutectic Solvents (DESs) are hygroscopic liquids composed of a hydrogen bond donor (HBD) and acceptor (HBA). Their physical, chemical and electrochemical properties can be tailored to use them as..., info:eu-repo/semantics/published
Published: 2020

44. Cellulose fibers modification through metal-free click chemistry for the elaboration of versatile functional surfaces

Author: Louise Hespel, Alex Myeye Biyogo, Vincent Humblot, Laurent Lebrun, François Estour, Laboratoire de Réactivité de Surface (LRS), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Chimie Organique et Bioorganique : Réactivité et Analyse (COBRA), Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie Organique Fine (IRCOF), Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Polymères Biopolymères Surfaces (PBS), Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Institut Normand de Chimie Moléculaire Médicinale et Macromoléculaire (INC3M), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Université Le Havre Normandie (ULH), Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Fluorophore, Polymers and Plastics, Chemistry, Organic Chemistry, General Physics and Astronomy, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Cellulose fiber, chemistry.chemical_compound, [CHIM.POLY]Chemical Sciences/Polymers, X-ray photoelectron spectroscopy, Covalent bond, Yield (chemistry), Polymer chemistry, Materials Chemistry, Click chemistry, Molecule, [CHIM]Chemical Sciences, Cellulose, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract: In the present work, a novel and versatile way was developed to functionalize cellulose fibers from wipes under heterogeneous conditions. The technic was based on metal-free click chemistry to avoid the persistence of any metal traces on cellulose. First, cellulose fibers were covalently pre-functionalized with bicyclononyne (BCN) to promoted azide-alkyne addition with molecules of interest, like coumarin and β-cyclodextrin derivatives. X-ray photoelectron microscopy (XPS) shows that one BCN group per cellulose unit was modified at the surface of the wipe. 3-azido-7-hydroxycoumarin that can be used as fluorophore for bio-sensoring applications was efficiently bound to the pre-functionalized cellulose with a yield of reaction estimated at 60%. The addition of 6-azido-per-6-deoxy-β-cyclodextrin (β-CD derivative) was investigated in order to target future organophosphorus decontamination properties to cellulose wipes. With the best reaction conditions, 60% of triazole groups corresponding to 4 reactive azido groups per β-CD derivative were detected by XPS proving the efficiency of the click reaction. The highest DS values were obtained after 96 h for β-CD 20 Eq (DS = 1.7 % by elementary analysis and DS = 2.5 % by weight measurements). Scanning electron microscopy observations highlighted a globally well distributed β-CD with some aggregates on the surface of the fibers. Thus, the pre-functionalized BCN-cellulose fibers could be used for many applications after an easy clicking of target compounds.
Published: 2020

45. In-Situ Energy Dispersive X-ray Reflectivity Applied to Polyoxometalate Films: An Approach to Morphology and Interface Stability Issues in Organic Photovoltaics

Author: Amanda Generosi, Barbara Paci, Anna Proust, Ludovic Tortech, Marco Guaragno, Qirong Zhu, Nicholas Barrett, Istituto di Struttura della Materia (CNR-ISM), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Etude des NanoStructures et Imagerie de Surface (LENSIS), Service de physique de l'état condensé (SPEC - UMR3680), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Région Ile de France/DIM Nano-K, Consiglio Nazionale delle Ricerche [Roma] (CNR), Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: Materials science, Physics and Astronomy (miscellaneous), Organic solar cell, in-situ X-ray characterization, General Mathematics, Interface (computing), time resolved EDXR, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Computer Science (miscellaneous), Thin film, business.industry, lcsh:Mathematics, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, lcsh:QA1-939, Durability, 0104 chemical sciences, X-ray reflectivity, Chemistry (miscellaneous), thin films structure and morphology, Polyoxometalate, Degradation (geology), Optoelectronics, polyoxymetalate functional materials, organic photovoltaics, 0210 nano-technology, business, Layer (electronics)
Abstract: Organic solar cells, characterized by a symmetrical regular layered structure, are very promising systems for developing green, low cost, and flexible solar energy conversion devices. Despite the efficiencies being appealing (over 17%), the technological transfer is still limited by the low durability. Several processes, in bulk and at interface, are responsible. The quick downgrading of the performance is due to a combination of physical and chemical degradations. These phenomena induce instability and a drop of performance in working conditions. Close monitoring of these processes is mandatory to understand the degradation pathways upon device operation. Here, an unconventional approach based on Energy Dispersive X-ray Reflectivity (ED-XRR) performed in-situ is used to address the role of Wells–Dawson polyoxometalate (K6-P2W18O62, hereafter K6-P2W18) as hole transporting layer in organic photovoltaics. The results demonstrate that K6-P2W18 thin films, showing ideal bulk and interface properties and superior optical/morphological stability upon prolonged illumination, are attractive candidates for the interface of durable OPV devices.
Published: 2020

46. Combining surface chemistry modification and in situ small-angle scattering characterization to understand and optimize the biological behavior of nanomedicines

Author: Marine Le Goas, Elodie Barruet, Maria Kalbazova, Tom Roussel, David Carriere, Jean Philippe Renault, Geraldine Carrot, Fabienne Testard, Valérie Geertsen, Giulia C Fadda, Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), UFR Santé, Médecine et Biologie Humaine (UFR SMBH), Université Sorbonne Paris Nord, ANR-11-IDEX-0003,IPS,Idex Paris-Saclay(2011), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay
Subjects: In situ, Cell Membrane Permeability, Surface Properties, Biomedical Engineering, Nanoparticle, Metal Nanoparticles, Nanotechnology, Antineoplastic Agents, Biocompatible Materials, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Small Molecule Libraries, Mice, Polymethacrylic Acids, Scattering, Small Angle, Animals, Humans, General Materials Science, Particle Size, Chemistry, General Chemistry, General Medicine, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Characterization (materials science), Cancer treatment, Nanomedicine, Colloidal gold, Gold, Small-angle scattering, 0210 nano-technology, Hydrophobic and Hydrophilic Interactions
Abstract: International audience; Nanomedicines are considered as promising therapeutics for cancer treatment. However, clinical translation is still scarce, partly because their biological behavior is not well understood. Extracting general guidelines from the great variety of nanoparticles and conditions studied is indeed difficult, and relevant techniques are lacking to obtain in situ information. Here, both issues are solved by combining versatile model nanoparticles with in situ tools based on small-angle scattering techniques (SAS). The strategy was to develop a library of nanoparticles and perform systematic study of their interactions with biological systems. Considering the promising properties of gold nanoparticles as cancer therapeutics, polymethacrylate-grafted gold nanoparticles were chosen as models. Modulation of polymer chemistry was shown to change the surface properties while keeping the same structure for all nanoparticles. This unity allowed reliable comparison to extract general principles, while the synthesis versatility enabled to fine-tune the nanoparticles surface properties, especially through copolymerization, and thus to optimize their biological behavior. Two specific aspects were particularly examined: colloidal stability and cell uptake. Positive charges and hydrophobicity were identified as key parameters influencing toxicity and internalization. In situ SAS gave valuable information about nanoparticles evolution in biologically relevant environments. Good colloidal stability was thereby shown in cell culture media, while intracellular transformation and quantity of nanoparticles were monitored, highlighting the potential of these techniques for nanomedicines studies.
Published: 2020
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47. Evaluation of particle and bed integrity of aqueous size-exclusion columns packed with sub-2 µm particles operated at high pressure

Author: Sebastiaan Eeltink, Mary J. Wirth, Jelle De Vos, Gino Baron, Herman Terryn, Erwin Kaal, Chemical Engineering and Separation Science, Chemical Engineering and Industrial Chemistry, Centre for Molecular Separation Science & Technology, Vriendenkring VUB, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: Void (astronomy), Scanning electron microscope, uhplc, Size-exclusion chromatography, BEH SEC particles, 010402 general chemistry, 01 natural sciences, Biochemistry, Analytical Chemistry, Protein analysis, Particle Size, Composite material, Chromatography, High Pressure Liquid, Pressure drop, Chromatography, Aqueous solution, Chemistry, 010401 analytical chemistry, Organic Chemistry, Proteins, Water, General Medicine, Porosimetry, 0104 chemical sciences, Volumetric flow rate, Column bed stability, Chromatography, Gel, Particle size
Abstract: The performance of columns packed with 1.7 µm particles for aqueous size-exclusion chromatography was assessed at high-pressure conditions and linked to particle- and column-bed integrity. Decreasing the particle size from 3.5 µm to 1.7 µm increases the resolution due to the improved mass-transfer characteristics, allowing to significantly speed-up analysis without compromising the selectivity. A sub-minute separation of intact proteins was realized on a 4.6 mm i.d × 75 mm long column packed with 1.7 µm SEC particles applying a flow rate of 1.8 mL/min, corresponding to a column pressure of 530 bar. Ultra-high pressure operation (exceeding manufacturer's recommendations) resulted in peak deformation, a shift towards earlier retention times, and an alteration in selectivity. To gain insights in the mechanisms of column deterioration, short 30 mm long columns were operated at UHPLC conditions, maximizing the pressure drop over individual particles. This resulted in the presence of fractured particles situated at the column outlet, as verified by scanning electron micrographs. Mercury-intrusion porosimetry and argon-adsorption measurements did not reveal significant differences in intraparticle volume between particle batches sampled before and after pressure stress testing. As particles at the column outlet fracture (but not collapse) at high pressure operation, a void was formed at the column inlet. The degradation of the separation performance appeared to be the result of a decrease in interparticle pore volume.
Published: 2020

48. ATR-FTIR in Kretschmann configuration integrated with electrochemical cell as in situ interfacial sensitive tool to study corrosion inhibitors for magnesium substrates

Author: Robert H. Meißner, Sviatlana V. Lamaka, Herman Terryn, R. Unbehau, Tim Würger, Johannes M. C. Mol, Mikhail L. Zheludkevich, B. Boelen, L.I. Fockaert, Materials and Surface Science & Engineering, Electrochemical and Surface Engineering, and Materials and Chemistry
Subjects: corrosion inhibitors, General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, chemisorption, magnesium, 010402 general chemistry, 01 natural sciences, DFT, chemistry.chemical_compound, Adsorption, integrated ATR-FTIR, Electrochemistry, Molecule, Carboxylate, Fourier transform infrared spectroscopy, Technik [600], ddc:620.11, Magnesium, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Dielectric spectroscopy, chemistry, Chemisorption, Attenuated total reflection, Chemical Engineering(all), 0210 nano-technology, EIS setup, ddc:600
Abstract: Integrated attenuated total reflection – Fourier transform infrared spectroscopy (ATR-FTIR) – Electrochemical impedance spectroscopy (EIS) measurements were used to simultaneously follow chemisorption mechanisms of organic inhibitors as well as their corrosion inhibition efficiency towards magnesium based substrates. Four carboxylic compounds, i.e. 2,5-pyridinedicarboxylic acid (PDC), 3-methylsalicylic acid (MSA), sodium salicylate (SS) and fumaric acid (FA), were selected based on their promising inhibiting capacities and were all shown to chemisorb at the MgO/Mg(OH)2 surface by carboxylate bond formation. Orientation analysis using polarized infrared light showed that carboxylate bonds established using aliphatic carboxylate compound aligned perpendicular to the magnesium surface, whereas carboxylate bonds with aromatic compounds were oriented in plane with the magnesium surface. This different orientation is associated to the involvement of π-interactions in the MgO/Mg(OH)2 – aromatic carboxylate adsorption. Additionally, DFT calculations revealed that the addition of hetero-atoms (i.e. N or OH) in the molecular structure contributes to increased adsorption energies, indicating that next to carboxylate groups also these hetero-atoms are involved in interfacial interactions. Integrating the ATR-FTIR setup with an electrochemical cell allowing for simultaneous EIS measurements lead to two surface phenomena determining the inhibition efficiency. Surface hydroxylation processes on one hand forming a MgO/Mg(OH)2 layer on one hand, and the chemisorption of carboxylate compounds on the other hand. The inhibition efficiency was found to increase in following order: FA < PDC < MSA and was mainly associated to the formation of a MgO/Mg(OH)2 layer. SS was shown to act as a corrosion accelerator rather than a corrosion inhibitor. Despite its high sensitivity for water, both surface processes could be followed in situ by means of ATR-FTIR. Simultaneously, protective properties of the formed films could be quantified by means of EIS. Consequently, integrated ATR-FTIR – EIS methodology has shown to be highly valuable for gaining in-situ insights in the inhibition mechanism, while quantifying the inhibition efficiency. This was even possible for highly active metal substrate as magnesium, although further developments are suggested if one aims to quantify electrochemical constants related to corrosion and other surface processes measured at the low frequencies (i.e. < 1 Hz).
Published: 2020

49. Oxygen reduction reaction catalyzed by overhanging carboxylic acid strapped iron porphyrins adsorbed on carbon nanotubes

Author: Hélène Arcostanzo, Pradip K. Das, Bernard Boitrel, Manel Hanana, Stéphane Campidelli, Morgane Bouget, Renaud Cornut, Bruno Jousselme, Stéphane Le Gac, Thierry Roisnel, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), ANR-14-JTIC-0002-01, TMOL 'Molecular Technology', ANR-16-CE29-0027-01, MAGMA, ANR-14-JTIC-0002,MECANO,Ingenierie moléculaire et assemblages contrôlés de nanoobjets fonctionnels à base de porphyrines(2014), ANR-16-CE29-0027,MAGMA,Propriétés Magnétiques du Graphène Fonctionnalisé par des Assemblages Moléculaires Bidimensionnels(2016), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Porphyrins, Proton, Carboxylic acid, Carbon nanotube, 010402 general chemistry, 01 natural sciences, Catalysis, law.invention, Synthesis, Adsorption, law, Polymer chemistry, Oxygen reduction reaction, heterocyclic compounds, chemistry.chemical_classification, dioxygen reduction, 010405 organic chemistry, Chemistry, [CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 0104 chemical sciences, X-ray diffraction, X-ray crystallography
Abstract: International audience; A series of hybrid catalysts for the oxygen reduction reaction (ORR) has been investigated. They are composed of multi-wall carbon nanotubes (MWNTs) coated with iron strapped porphyrins. Two porphyrins have been probed; both are strapped with the same skeleton and differ only by the number of overhung carboxylic acid(s), either one or two. In this structure, the carboxylic acid group can act as a proton relay between the medium and the catalyst or as a polar group surrounding the dioxygen binding cavity. While the number of carboxylic acid group(s) does not exhibit a significant influence on the catalytic properties, the combination of both components–MWNTs and porphyrin–leads to a better catalytic activity than those of the nanotubes or the porphyrins taken separately.
Published: 2020

50. A soft-chemistry assisted strong metal–support interaction on a designed plasmonic core–shell photocatalyst for enhanced photocatalytic hydrogen production

Author: Robert Wojcieszak, Hynd Remita, Getaneh Diress Gesesse, Cong Wang, Shih Hsuan Tai, Christophe Colbeau-Justin, Patricia Beaunier, Bor Kae Chang, Mohamed Nawfal Ghazzal, Université Paris-Saclay, Laboratoire de Chimie Physique D'Orsay (LCPO), Université Paris-Sud - Paris 11 (UP11)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Laboratoire de Physique des Surfaces et des Interfaces (LPSI), Université de Mons-Hainaut, Institut de Chimie Physique (ICP), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Université de Lille, CNRS, Centrale Lille, ENSCL, Univ. Artois, and Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Subjects: Materials science, Hydrogen, chemistry.chemical_element, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, Soft chemistry, 0104 chemical sciences, Overlayer, Chemical engineering, chemistry, Colloidal gold, Photocatalysis, [CHIM]Chemical Sciences, General Materials Science, Density functional theory, 0210 nano-technology, Plasmon, ComputingMilieux_MISCELLANEOUS, Hydrogen production
Abstract: Engineering photocatalysts based on gold nanoparticles (AuNPs) has attracted great attention for the solar energy conversion due to their multiple and unique properties. However, boosting the photocatalytic performance of plasmonic materials for H2 generation has some limitations. In this study, we propose a soft-chemistry method for the preparation of a strong metal–support interaction (SMSI) to enhance the photocatalytic production of H2. The TiO2 thin overlayer covering finely dispersed AuNPs (forming an SMSI) boosts the photocatalytic generation of hydrogen, compared to AuNPs deposited at the surface of TiO2 (labelled as a classical system). The pathway of the charge carriers’ dynamics regarding the system configuration is found to be different. The photogenerated electrons are collected by AuNPs in a classical system and act as an active site, while, unconventionally, they are injected back in the titania surface for an SMSI photocatalyst making the system highly efficient. Additionally, the adsorption energy of methanol, theoretically estimated using the density functional theory (DFT) methodology, is lower for the soft-chemistry SMSI photocatalyst accelerating the kinetics of photocatalytic hydrogen production. The SMSI obtained by soft-chemistry is an original concept for highly efficient photocatalytic materials, where the photon-to-energy conversion remains a major challenge. 12
Published: 2020

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