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1. Hydrogen Production at a NiO Photocathode Based on a Ruthenium Dye-Cobalt Diimine Dioxime Catalyst Assembly: Insights from Advanced Spectroscopy and Post-operando Characterization

Author

Didier Gasparutto, Benjamin Dietzek, Alexander Schwab, Murielle Chavarot-Kerlidou, Stephan Kupfer, Didier Léonard, Christine Saint-Pierre, Sebastian Bold, Nicolas Queyriaux, Jakob Bruhnke, Carolin Müller, Emmanouil Giannoudis, Vincent Artero, Dmitry Aldakov, Corinne Gablin, 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), Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich-Schiller-Universität = Friedrich Schiller University Jena [Jena, Germany], Department Functional Interfaces, Leibniz Institute of Photonic Technology Jena (IPHT), Center for Energy and Environmental Chemistry (CEEC Jena), Institut des Sciences Analytiques (ISA), 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), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Leibniz Institute of Photonic Technology Jena, Department Functional Interfaces, Albert-Einstein-Straße 9, 07745 Jena, Germany, Institute of Physical Chemistry and Center for Energy and Environmental Chemistry Jena, (CEEC- Jena), Surfaces, Centre National de la Recherche Scientifique (CNRS)-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon, Institute for Physical Chemistry and Center for Energy and Environmental Chemistry, This work was supported by the European Commission's Seventh Framework Program (FP7/2007-2013) under grant agreement no. 306398 (FP7-IDEAS-ERC, Project PhotocatH2ode), the Deutsche Forschungsgemeinschaft (German Science Foundation, PHOTOACC project, grant no. KU 3933/2-1), and the French National Research Agency in the framework of the 'Investissements d'avenir' program (ANR15-IDEX-02, Labex ARCANE and CBH-EURGS, ANR-17EURE-0003) and the Franco-German University., ANR-11-LABX-0003,ARCANE,Grenoble, une chimie bio-motivée(2011), European Project: 306398,EC:FP7:ERC,ERC-2012-StG_20111012,PHOTOCATH2ODE(2012), Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)

Subjects
dye-sensitized, Materials science, Hydrogen, solar fuels, Photoelectrochemistry, chemistry.chemical_element, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Photochemistry, 7. Clean energy, 01 natural sciences, Catalysis, Artificial photosynthesis, photoelectrochemistry, cobalt catalyst, General Materials Science, Hydrogen production, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, Solar fuel, 0104 chemical sciences, Ruthenium, chemistry, 13. Climate action, hydrogen, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Water splitting, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other
Abstract

International audience; The production of hydrogen by efficient, low-cost, and integrated photoelectrochemical water splitting processes represents an important target for the ecological transition. This challenge can be addressed thanks to bioinspired chemistry and artificial photosynthesis approaches by designing dye-sensitized photocathodes for hydrogen production, incorporating bioinspired first-row transition metal-based catalysts. The present work r describes the preparation and photoelectrochemical characterization of a NiO photocathode sensitized with a phosphonate-derivatized ruthenium tris-diimine photosensitizer covalently linked to a cobalt diimine dioxime hydrogen-evolving catalyst. Under simulated AM 1.5G irradiation, hydrogen is produced with photocurrent densities reaching 84 +/- 7 mu A.cm(-2), which is among the highest values reported so far for dye-sensitized photocathodes with surface-immobilized catalysts. Thanks to the unique combination of advanced spectroscopy and surface characterization techniques, the fast desorption of the dyad from the NiO electrode and the low yield of electron transfer to the catalyst, resulting in the Co demetallation from the diimine dioxime framework, were identified as the main barriers limiting the performances and the stability of the system. This work therefore paves the way for a more rational design of molecular photocathodes for solar fuel production and represents a further step toward the development of sustainable processes for the production of hydrogen from sunlight and water.

Published
2021
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2. Roadmap on dynamics of molecules and clusters in the gas phase

Author

Claire Romanzin, Alicja Domaracka, S. D. Tošić, Michael Gatchell, Jaroslav Kočišek, Simon Albertini, Mattea Carmen Castrovilli, Steen Brøndsted Nielsen, Ewa Erdmann, Janina Kopyra, Sylvain Maclot, Daniela Ascenzi, Amanda L. Steber, Klavs Hansen, Marta Łabuda, Christophe Jouvet, Lars H. Andersen, Dariusz G. Piekarski, Manuel Alcamí, Alicia Palacios, Sergio Díaz-Tendero, Henrik Cederquist, Elisabeth Gruber, Lorenzo Avaldi, Paola Bolognesi, Per Johnsson, Yoni Toker, Shirin Faraji, Oded Heber, Annemieke Petrignani, Christina Kjær, A. Candian, Aleksandar R. Milosavljević, Jennifer A. Noble, Paulo Limão-Vieira, Patrick Rousseau, Henning T. Schmidt, Eduardo Carrascosa, Juraj Fedor, Denis S. Tikhonov, Thomas Schlathölter, James N. Bull, Sadia Bari, Henning Zettergren, Department of Physics [Stockholm], Stockholm University, Centre de recherche sur les Ions, les MAtériaux et la Photonique (CIMAP - UMR 6252), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-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), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Zernike Institute for Advanced Materials, University of Groningen [Groningen], Istituto di Struttura della Materia (CNR-ISM), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Departamento de Química, Módulo 13, Universidad Autónoma de Madrid, 28049 Madrid (Spain), Department of Theoretical Physics and Quantum Information (DTPQI), ‎ Gdansk University of technology, Institute of Physics [Belgrade], University of Belgrade [Belgrade], Department of Physics (Göthenburg), University of Gothenburg (GU), Department of Physics, Mathematical Physics [Lund], Lund University [Lund], Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Departamento de Química, Modulo 13, Universidad Autónoma de Madrid, Universidad Autónoma de Madrid (UAM), Institute of Physical Chemistry [Warsaw], Polish Academy of Sciences, Department III, Normandie Université (NU), Department of Physics (DPUT), University of Trento [Trento], Institut de Chimie Physique (ICP), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Siedlce University of Natural Sciences and Humanities, Centro de Física e Investigação Tecnológica [Lisboa] (CEFITEC), Departamento de Fìsica [Lisboa] (DF), Faculdade de Ciências e Tecnologia = School of Science & Technology (FCT NOVA), Universidade Nova de Lisboa = NOVA University Lisbon (NOVA)-Universidade Nova de Lisboa = NOVA University Lisbon (NOVA)-Faculdade de Ciências e Tecnologia = School of Science & Technology (FCT NOVA), Universidade Nova de Lisboa = NOVA University Lisbon (NOVA)-Universidade Nova de Lisboa = NOVA University Lisbon (NOVA), J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Institut für Ionenphysik und Angewandte Physik - Institute for Ion Physics and Applied Physics [Innsbruck], Leopold Franzens Universität Innsbruck - University of Innsbruck, Department of Physics and Astronomy [Aarhus], Aarhus University [Aarhus], Department of Particle Physics, Weizmann Institute of Science, Ajo, Bar-Ilan University [Israël], Tianjin University of Science and Technology (TUST), Physique des interactions ioniques et moléculaires (PIIM), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Ecole Polytechnique Fédérale de Lausanne (EPFL), University of East Anglia [Norwich] (UEA), van ‘t Hoff Institute for Molecular Sciences, Universiteit van Amsterdam (UvA), DF – Departamento de Física, CeFITec – Centro de Física e Investigação Tecnológica, UAM. Departamento de Química, Molecular Processes Modeling Group, Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Caen Normandie (UNICAEN), Consiglio Nazionale delle Ricerche [Roma] (CNR), Universidad Autonoma de Madrid (UAM), School of Chemistry, University of East Anglia, Norwich Research Park, Norwich NR4 7TJ, United Kingdom, Van't Hoff Institute for Molecular Sciences, University of Amsterdam [Amsterdam] (UvA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Quantum interactions and structural dynamics, and Theoretical Chemistry

Subjects
ab-initio, Astrochemistry, cold ion spectroscopy, COLD ION SPECTROSCOPY, storage-ring, Clusters in the Gas Phase, Nanotechnology, 02 engineering and technology, Physics, Atomic, Molecular & Chemical, 010402 general chemistry, 01 natural sciences, Gas phase, POLYCYCLIC AROMATIC-HYDROCARBONS, resolved photoelectron-spectroscopy, fragmentation dynamics, Molecule, ddc:530, STORAGE-RING, THERMIONIC EMISSION, AB-INITIO, Physics, polycyclic aromatic-hydrocarbons, Science & Technology, low-energy electrons, LOW-ENERGY ELECTRONS, FRAGMENTATION DYNAMICS, RESOLVED PHOTOELECTRON-SPECTROSCOPY, [PHYS.PHYS.PHYS-ATM-PH]Physics [physics]/Physics [physics]/Atomic and Molecular Clusters [physics.atm-clus], Optics, SUPERFLUID-HELIUM DROPLETS, MASS-SPECTROMETRY, Química, mass-spectrometry, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Dynamics of Molecules, superfluid-helium droplets, Physical Sciences, thermionic emission, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 0210 nano-technology
Abstract

The European physical journal / D 75(5), 152 (2021). doi:10.1140/epjd/s10053-021-00155-y, This roadmap article highlights recent advances, challenges and future prospects in studies of the dynamics of molecules and clusters in the gas phase. It comprises nineteen contributions by scientists with leading expertise in complementary experimental and theoretical techniques to probe the dynamics on timescales spanning twenty order of magnitudes, from attoseconds to minutes and beyond, and for systems ranging in complexity from the smallest (diatomic) molecules to clusters and nanoparticles. Combining some of these techniques opens up new avenues to unravel hitherto unexplored reaction pathways and mechanisms, and to establish their significance in, e.g. radiotherapy and radiation damage on the nanoscale, astrophysics, astrochemistry and atmospheric science., Published by Springer, Heidelberg

Published
2021
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3. Mechanochemical Forces as a Synthetic Tool for Zero- and One-Dimensional Titanium Oxide-Based Nano-photocatalysts

Author

Dimitrios A. Giannakoudakis, Juan Carlos Colmenares, Gregory Chatel, Institute of Physical Chemistry Polish Academy of Sciences, Laboratoire de Chimie Moléculaire et Environnement (LCME), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Institute of Physical Chemistry, Polish Academy of Sciences, and Polska Akademia Nauk = Polish Academy of Sciences (PAN)

Subjects
Solid-state chemistry, Nanotechnology, Review, 02 engineering and technology, 010402 general chemistry, Sonochimie, 01 natural sciences, Catalysis, Nanomaterials, Sonochemistry, chemistry.chemical_compound, Ball milling, Mechanochemistry, Nano, Ultrasound-assisted synthesis, Photocatalyse, [CHIM]Chemical Sciences, Photocatalysis, Synthèse assistée par ultrasons, Titanium, Méchanochimie, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, Photochemical Processes, 021001 nanoscience & nanotechnology, One-dimensional titanium oxide, 0104 chemical sciences, Titanium oxide, chemistry, Titanium dioxide, Nanoparticles, 0210 nano-technology
Abstract

Abstract A new field where the utilization of mechanochemistry can create new opportunities is materials chemistry, and, more interestingly, the synthesis of novel nanomaterials. Ball-milling procedures and ultrasonic techniques can be regarded as the most important mechanochemical synthetic tools, since they can act as attractive alternatives to the conventional methods. It is also feasible for the utilization of mechanochemical forces to act synergistically with the conventional synthesis (as a pre-treatment step, or simultaneously during the synthesis) in order to improve the synthetic process and/or the material’s desired features. The usage of ultrasound irradiation or ball-milling treatment is found to play a crucial role in controlling and enhancing the structural, morphological, optical, and surface chemistry features that are important for heterogeneous photocatalytic practices. The focus of this article is to collect all the available examples in which the utilization of sonochemistry or ball milling had unique effects as a synthesis tool towards zero- or one-dimensional nanostructures of a semiconductor which is assumed as a benchmark in photocatalysis, titanium dioxide. Graphical Abstract

Published
2020
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4. Structure of Ni(OH) 2 intermediates determines the efficiency of NiO-based photocathodes – a case study using novel mesoporous NiO nanostars

Author

Markus Rettenmayr, Christa Schmidt, Vincent Artero, Jan Dellith, Jennifer Fize, Ruri Agung Wahyuono, Murielle Chavarot-Kerlidou, Benjamin Dietzek, Andrea Dellith, Anna Ignaszak, Martin Seyring, Leibniz Institute of Photonic Technology Jena, Department Functional Interfaces, Albert-Einstein-Straße 9, 07745 Jena, Germany, Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich-Schiller-Universität = Friedrich Schiller University Jena [Jena, Germany], Department of Chemistry, University of New Brunswick, Otto-Schott-Institute of Materials Research (OSIM), 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 [2016-2019] (UGA [2016-2019])-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 [2016-2019] (UGA [2016-2019]), Center for Energy and Environmental Chemistry (CEEC Jena), Institute of Physical Chemistry, Abbe Center of Photonics, Friedrich-Schiller-Universität Jena, Centre National de la Recherche Scientifique (CNRS)-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)-Centre National de la Recherche Scientifique (CNRS)-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), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG)

Subjects
chemistry.chemical_classification, Photocurrent, Materials science, Band gap, General Chemical Engineering, Non-blocking I/O, Nanoparticle, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, General Chemistry, Electron acceptor, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, Photocathode, 0104 chemical sciences, chemistry, Specific surface area, [CHIM.COOR]Chemical Sciences/Coordination chemistry, 0210 nano-technology, Mesoporous material
Abstract

International audience; We report the wet chemical synthesis of mesoporous NiO nanostars (NS) as photocathode material for dye-sensitized solar cells (DSSCs). The growth mechanism of NiO NS as a new morphology of NiO is assessed by TEM and spectroscopic investigations. The NiO NS are obtained upon annealing of preformed beta-Ni(OH)(2) into pristine NiO with low defect concentrations and favorable electronic configuration for dye sensitization. The NiO NS consist of fibers self-assembled from nanoparticles yielding a specific surface area of 44.9 m(2) g(-1). They possess a band gap of 3.83 eV and can be sensitized by molecular photosensitizers bearing a range of anchoring groups, e.g. carboxylic acid, phosphonic acid, and pyridine. The performance of NiO NS-based photocathodes in photoelectrochemical application is compared to that of other NiO morphologies, i.e. nanoparticles and nanoflakes, under identical conditions. Sensitization of NiO NS with the benchmark organic dye P1 leads to p-DSSCs with a high photocurrent up to 3.91 mA cm(-2) whilst the photoelectrochemical activity of the NiO NS photocathode in aqueous medium in the presence of an irreversible electron acceptor is reflected by generation of a photocurrent up to 23 mu A cm(-2).

Published
2019
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5. Investigating Light-Driven Hole Injection and Hydrogen EvolutionCatalysis at Dye-Sensitized NiO Photocathodes: A CombinedExperimental−Theoretical Study

Author

Murielle Chavarot-Kerlidou, Julien Massin, Vincent Artero, Michele Pavone, Sebastian Bold, Maximilian Bräutigam, Benjamin Dietzek, Maria Wächtler, Ana B. Muñoz-García, 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 [2016-2019] (UGA [2016-2019])-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 [2016-2019] (UGA [2016-2019]), Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich-Schiller-Universität = Friedrich Schiller University Jena [Jena, Germany], Leibniz Institute of Photonic Technology Jena, Department Functional Interfaces, Albert-Einstein-Straße 9, 07745 Jena, Germany, Department of Chemical Sciences, University of Naples Federico II, Dipartimento di Fisica 'Ettore Pancini', Università degli studi di Napoli Federico II, Institute for Physical Chemistry and Center for Energy and Environmental Chemistry, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-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), University of Naples Federico II = Università degli studi di Napoli Federico II, ANR-17-EURE-0003,CBH-EUR-GS,CBH-EUR-GS(2017), Massin, J., Brautigam, M., Bold, S., Wachtler, M., Pavone, M., Munoz-Garcia, A. B., Dietzek, B., Artero, V., and Chavarot-Kerlidou, M.

Subjects
Materials science, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Quantum chemistry, Photocathode, Catalysis, Metal, Electron transfer, Ultrafast laser spectroscopy, Physical and Theoretical Chemistry, business.industry, Non-blocking I/O, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Solar energy, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Energy, visual_art, visual_art.visual_art_medium, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optoelectronics, 0210 nano-technology, business
Abstract

International audience; Dye-sensitized photoelectrochemical cells form an emerging technology for the large-scale storage of solar energy in the form of (solar) fuels because of the low cost and easy processing of their constitutive photoelectrode materials. Such hybrid photoelectrodes consist of molecular dyes grafted onto transparent semiconducting metal oxides in combination with catalytic centers. The optimization of the performances of such hybrid photoelectrodes requires a detailed understanding of the light-driven electron transfer processes occurring first at the interface between the semiconducting material and the dye and then between the dye and the catalytic center. Here we address the first of these issues and use quantum chemistry to determine the structural and electronic features of the interfaces between a push-pull dye and the p-NiO (100) surface. We show that these calculations are in good agreement with transient absorption spectroscopic measurements on a prototypical dye-sensitized photocathode system able to evolve hydrogen in the presence of a cobaloxime catalyst in solution.

Published
2019
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6. Effect of insoluble surfactants on a thermocapillary flow

Author

Pierre Lambert, Aude Bolopion, Franco Nicolas Pinan Basualdo, Benoit Scheid, Michaël Gauthier, R. Terrazas Mallea, Franche-Comté Électronique Mécanique, Thermique et Optique - Sciences et Technologies (UMR 6174) (FEMTO-ST), Université de Technologie de Belfort-Montbeliard (UTBM)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Université de Franche-Comté (UFC), Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC)-Centre National de la Recherche Scientifique (CNRS), Institute of Physical Chemistry, Polish Academy of Sciences, (Institute of Physical Chemistry,), Université libre de Bruxelles (ULB), and Department of Bio, Electro And Mechanical Systems (BEAMS)

Subjects
Work (thermodynamics), Mécanique des fluides, [INFO.INFO-DS]Computer Science [cs]/Data Structures and Algorithms [cs.DS], Microfluidics, Flow (psychology), Computational Mechanics, 02 engineering and technology, Sciences de l'ingénieur, 01 natural sciences, [SPI.AUTO]Engineering Sciences [physics]/Automatic, 010305 fluids & plasmas, Physics::Fluid Dynamics, Particle tracking velocimetry, 0103 physical sciences, Miniaturization, Convection cell, Fluid Flow and Transfer Processes, Physics, Mechanical Engineering, Mechanics, Radius, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Temperature gradient, Mechanics of Materials, 0210 nano-technology
Abstract

International audience; The thermocapillary effect, arising flow due to a temperature gradient along a fluid interface, is the dominant effect in some industrial and microfluidics processes and must be studied in order to optimise them. In this work, we analyse how insoluble surfactants adsorbed at the interface can affect such a flow. In particular, we analyse the case where the thermocapillary flow is induced at the air-water interface by locally heating it with an infrared laser, setup that is used to manipulate floating particles through the generated flow. Since water is a polar fluid, the air-water interface is easily polluted by surfactants. We developed a numerical model considering the uncontrolled presence of surfactants, which evidences that the effect of the surface contamination cannot be neglected, even for small surfactants concentration. The results of this numerical model were compared with different experimental measurements: particle tracking velocimetry, convection cell radius measurements and thermography of the surface. All the experimental observations agree with the numerical model with the initial surface contamination being a fitting parameter. The model was then validated comparing its results with measurements for which a known quantity of surfactant was added to the interface. Finally, an analytical model was developed to explain the effects of the governing parameters, which agrees with the simulations and the experimental results. The developed models give us insights towards the miniaturization of the manipulation platform

Published
2021
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7. Influence of pretreatment and reaction conditions on the catalytic activity of HAlBEA and CoHAlBEA zeolites in vinyl chloride formation from 1,2-dichloroethane

Author

Yannick Millot, Anna Śrębowata, Christophe Calers, Stanislaw Dzwigaj, Emil Kowalewski, Dmytro Lisovytskiy, Laetitia Valentin, Izabela Kaminska, Institute of Physical Chemistry Polish Academy of Sciences, Institute of Physical Chemistry, PAS, Laboratoire de Réactivité de Surface (LRS), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chloride, Co BEA, 02 engineering and technology, 1,2-Dichloroethane, Dehydrochlorination, 010402 general chemistry, 01 natural sciences, Vinyl chloride, Catalysis, chemistry.chemical_compound, Physisorption, [CHIM]Chemical Sciences, General Materials Science, Zeolite, Chemistry, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Monomer, Mechanics of Materials, 2-Dichloroethane, 0210 nano-technology, Brønsted–Lowry acid–base theory, Selectivity, Vinyl, Nuclear chemistry
Abstract

International audience; HAlBEA and CoHAlBEA zeolite catalysts treated at 523 K or 873 K for 3 h in Ar, H2/Ar or air flows, respectively, were investigated in catalytic dehydrochlorination of 1,2-dichloroethane (DCE). The dehydrochlorination of DCE on these zeolite catalysts resulted in almost 100% selectivity to vinyl chloride (VC) monomer. It was demonstrated that different conditions of pretreatment of zeolite catalysts resulted in varied amount of Lewis and Brønsted acid sites responsible of the catalytic activity, stability and selectivity. HAlBEA and CoHAlBEA zeolites treated in the Ar flow showed the best activities in the dehydrochlorination of DCE, while the same zeolites treated in the air flow demonstrated the best time-on-stream stability. To clarify the reasons of differences in the catalytic behavior of HAlBEA and CoHAlBEA treated in the various conditions N2 physisorption, XRD, TPH, TEM, XPS, NMR and FTIR measurements were performed.

Published
2018
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8. Catalytic properties of AgAlBEA and AgSiBEA zeolites in H 2 -promoted selective reduction of NO with ethanol

Author

S. M. Orlyk, Stanislaw Dzwigaj, Sergiy O. Soloviev, Pavlo I. Kyriienko, Nataliia Popovych, L.V. Pisarzhevskii Institute of Physical Chemistry, National Academy of Sciences of Ukraine (NASU), L.V. Pisarzhevsky Institute of Physical Chemistry of the NAS of Ukraine, Laboratoire de Réactivité de Surface (LRS), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Silver, Hydrogen, Inorganic chemistry, chemistry.chemical_element, Infrared spectroscopy, 02 engineering and technology, 010402 general chemistry, Photochemistry, 7. Clean energy, 01 natural sciences, Catalysis, Nanoclusters, chemistry.chemical_compound, X-ray photoelectron spectroscopy, SCR of NO, Pyridine, [CHIM]Chemical Sciences, General Materials Science, Selective reduction, Hydrogen effect, Ethanol, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, chemistry, Mechanics of Materials, BEA zeolite, 0210 nano-technology
Abstract

International audience; Physicochemical properties of AgAlBEA and AgSiBEA zeolites were investigated by IR spectroscopy with pyridine, H2-TPR, XPS and diffuse reflectance UV–vis spectroscopy. Their catalytic properties were studied in the process of selective reduction of NO with ethanol and in the presence of hydrogen in reaction mixture. AgAlBEA catalysts show wider temperature range of NO-to-N2 conversion in the process of SCR with ethanol than AgSiBEA. Promoting H2-effect on the SCR of NO with ethanol is observed in the presence of AgAlBEA catalysts, whereas it is almost absent for AgSiBEA. A key factor for better performance of AgAlBEA than AgSiBEA is the presence of silver nanoclusters in close proximity of strong Lewis acidic sites.

Published
2015
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9. Photosensitized Degradation of Model Lipid Membranes based on 1-palmitoyl-2-oleyl-phosphatidylcholine (POPC)

Author

Alexander V. Shokurov, S. L. Selektor, Touria Cohen-Bouhacina, M. A. Grin, D. N. Novak, A. V. Zaytseva, Christine Grauby-Heywang, Vladimir V. Arslanov, A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences [Moscow] (RAS), Moscow State Technological University (MSTU Stankin), Laboratoire Ondes et Matière d'Aquitaine (LOMA), Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Russian Foundation for Basic research (project no. 177-53-150013 CNRS_a, CNRS project no. 1520, Centre National de la Recherche Scientifique (CNRS)-Université de Bordeaux (UB), and Frumkin Institute of Physical Chemistry and Electrochemistry (RAS)

Subjects
0301 basic medicine, 030103 biophysics, [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], Context (language use), 02 engineering and technology, Contact angle, 03 medical and health sciences, chemistry.chemical_compound, Phosphatidylcholine, Monolayer, Materials Chemistry, Photosensitizer, [SDV.BBM.BC]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Biochemistry [q-bio.BM], POPC, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], [PHYS.PHYS]Physics [physics]/Physics [physics], Organic Chemistry, technology, industry, and agriculture, Metals and Alloys, Biological membrane, 021001 nanoscience & nanotechnology, Surfaces, Coatings and Films, Membrane, chemistry, Biophysics, lipids (amino acids, peptides, and proteins), 0210 nano-technology
Abstract

International audience; In this work, we study the interaction of a well-known photosensitizer, MePha, with models of biological membrane (Langmuir monolayers and Langmuir–Schaeffer planar bilayers) based on one of the most important natural lipid, POPC, for the subsequent investigation of photodestruction processes in a context of photodynamic therapy treatment. Changes of macroscopic properties and morphology of POPC/MePha model membranes upon irradiation by visible light are recorded by means of contact angle measurements and atomic force microscopy, demonstrating clearly the possibility to use these methods for the study of photodestruction of artificial lipid membranes on solid substrates, but also for a comparative study of the efficiency of novel photosensitizers.

Published
2018
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10. Spectroscopy of jet-cooled methane in the lower icosad region: Empirical assignments of low-J″ spectral lines from two-temperature analysis

Author

Petr Pracna, Alain Campargue, Samir Kassi, Milan Mašát, Ondrej Votava, Didier Mondelain, J. Heyrosky´ Institute of Physical Chemistry (IPC), Czech Academy of Sciences [Prague] (CAS), J. Heyrovsky institute of Physical Chemistry, J. Heyrovsky Institute of Physical Chemistry, LAsers, Molécules et Environnement (LAME-LIPhy), Laboratoire Interdisciplinaire de Physique [Saint Martin d’Hères] (LIPhy), and Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)

Subjects
[PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Jet (fluid), Materials science, 010304 chemical physics, Spectrometer, 02 engineering and technology, 021001 nanoscience & nanotechnology, Quantum number, 01 natural sciences, Atomic and Molecular Physics, and Optics, Spectral line, Nuclear magnetic resonance, 0103 physical sciences, Supersonic speed, Physical and Theoretical Chemistry, Atomic physics, 0210 nano-technology, Absorption (electromagnetic radiation), Spectroscopy, Tunable laser
Abstract

International audience; Complete 12CH4 spectrum in the lower icosad spectral range (7050-7350 cm‑1) has been measured in supersonic jet at 28 K for the first time using direct absorption tunable diode laser spectrometer. Due to efficient rotational cooling only spectral lines with lower rotational quantum number J < 4 are observed in the spectrum. Spectral lines in the supersonic jet spectra have been matched with those in liquid nitrogen cooled cell spectra (81 K) and two-temperature method for empirical lower state rotational quantum number assignments has been applied to obtain accurate experimental values of the lower state rotational quantum numbers J″. Especially positions of lines with of J″ = 0 are relevant for vibrational band origin determination, as they are unambiguously the R(0) transitions of the respective bands.

Published
2013
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11. Electropolymerization of magnesium 5,15-di(n-methoxyphenyl)porphine

Author

Mikhail A. Vorotyntsev, I. P. Kalashnikova, V. E. Baulin, Charles H. Devillers, Dmitry V. Konev, K. V. Lizgina, O. I. Istakova, Institute of Problems of Chemical Physics, Russian Academy of Sciences [Moscow] ( RAS ), Mendeleev University of Chemical Technology of Russia, Department of Chemistry, M. V. Lomonosov Moscow State University, Lomonosov Moscow State University ( MSU ), Institute of Physiologically Active Compounds, Russian Academy of Sciences - Chernogolovka, Frumkin Institute of Physical Chemistry and Electrochemistry, Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] ( ICMUB ), Université de Bourgogne ( UB ) -Centre National de la Recherche Scientifique ( CNRS ), Russian Science Foundation 14-13-01244, Russian Academy of Sciences [Moscow] (RAS), Department of Chemistry, Lomonosov Moscow State University, Lomonosov Moscow State University (MSU), A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), and Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
conjugated polymer, oxidation, chemistry.chemical_element, polyporphine, 02 engineering and technology, fabrication, 010402 general chemistry, Photochemistry, Electrochemistry, 01 natural sciences, [ CHIM ] Chemical Sciences, chemistry.chemical_compound, porphine, mg(ii), Polymer chemistry, electroactive materials, [CHIM]Chemical Sciences, polymers, chemistry.chemical_classification, Magnesium, electropolymerization, Polymer, 021001 nanoscience & nanotechnology, 0104 chemical sciences, 3. Good health, Electroactive materials, 15-substituted porphine, Monomer, Cruciform, chemistry, Polymerization, ion, 0210 nano-technology, unsubstituted porphine, porphyrin
Abstract

International audience; The process of electroxidative polymerization of magnesium 5,15-di(N-methoxyphenyl)porphine MgP(MeOPh)(2) is studied. The presence of substituents in positions 5 and 15 of the porphine macroring makes reactive two of its four meso positions, which allows new bonds to be formed only in the opposite positions 10 and 20. As a result, the process of electropolymerization of this substituted monomer at its oxidation can produce only linear chains, in contrast to unsubstituted magnesium porphine MgP for which the polymer structure can both be linear and contain zigzag and/or cruciform fragments.

Published
2016
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12. A metal-responsive interdigitated bilayer for selective quantification of mercury( ii ) traces by surface plasmon resonance

Author

S.L. Selector, Michel Meyer, Roger Guilard, Alexander V. Shokurov, Alla Bessmertnykh-Lemeune, O. A. Raitman, Vladimir V. Arslanov, Aslan Yu. Tsivadze, Elizaveta V. Ermakova, Maria A. Kalinina, A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences [Moscow] (RAS), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), Centre National de la Recherche Scientifique (CNRS)-Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC), Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences [Moscow] ( RAS ), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] ( ICMUB ), and Université de Bourgogne ( UB ) -Centre National de la Recherche Scientifique ( CNRS )

Subjects
aqueous-solution, water, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, [ CHIM ] Chemical Sciences, 01 natural sciences, Biochemistry, Analytical Chemistry, Ion, sensor, optical-detection, Monolayer, Amphiphile, voltammetric determination, Electrochemistry, Environmental Chemistry, [CHIM]Chemical Sciences, Chelation, Surface plasmon resonance, Spectroscopy, impedance spectroscopy, Bilayer, self-assembled monolayers, spr, gold, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Mercury (element), chemistry, ions, 0210 nano-technology
Abstract

Reusable surface plasmon resonance chips allowing the quantitative and selective detection of mercury(II) ions in water at the 0.01 nM level are reported. The surface-modified gold sensor consists of a rarefied self-assembled monolayer of octanethiol topped with a Langmuir–Blodgett monolayer of an amphiphilic and highly-specific chelator. The interdigitated architecture confers to the bilayer a high packing density, surface coverage, and binding-group accessibility.

Published
2016
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13. Impact of molecular structure of polymer in 193 nm resist performance

Author

Christophe Brault, Cyril Brochon, Raluca Tiron, Esma Ismailova, Georges Hadziioannou, Damien Perret, Guy Schlatter, Christos L. Chochos, Claire Sourd, Philippe Bandelier, Christophe A. Serra, Laboratoire d'Ingenierie des Polymères pour les Hautes Technologies, Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), QuantECA - Circuits électroniques quantiques Alpes, Institut Néel (NEEL), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF), Institute of Physical Chemistry 'Demokritos' (IPC), National Center for Scientific Research 'Demokritos' (NCSR), Laboratoire d'Electronique et des Technologies de l'Information (CEA-LETI), Université Grenoble Alpes (UGA)-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), Lithography Laboratory, Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Rohm et Haas Electronic Materials, Ecole nationale supérieure de chimie, polymères et materiaux de strasbourg (ECPM), Commissariat à l'énergie atomique et aux énergies alternatives - Laboratoire d'Electronique et de Technologie de l'Information (CEA-LETI), Direction de Recherche Technologique (CEA) (DRT (CEA)), Laboratoire de Chimie des Polymères Organiques (LCPO), Université de Bordeaux (UB)-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Team 4 LCPO : Polymer Materials for Electronic, Energy, Information and Communication Technologies, Université de Bordeaux (UB)-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Bordeaux (UB)-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique ( CNRS ) -Université Louis Pasteur - Strasbourg I, NanoSpin - Nanospintronique et Transport Moléculaire, Institut Néel ( NEEL ), Centre National de la Recherche Scientifique ( CNRS ) -Université Grenoble Alpes [Saint Martin d'Hères]-Centre National de la Recherche Scientifique ( CNRS ) -Université Grenoble Alpes [Saint Martin d'Hères], Institute of Physical Chemistry 'Demokritos' ( IPC ), National Center for Scientific Research 'Demokritos' ( NCSR ), Laboratoire d'Electronique et des Technologies de l'Information ( CEA-LETI ), Commissariat à l'énergie atomique et aux énergies alternatives ( CEA ) -Université Grenoble Alpes [Saint Martin d'Hères], Commissariat à l'énergie atomique et aux énergies alternatives ( CEA ), Circuits électroniques quantiques Alpes (QuantECA), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF), Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC), Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC), Circuits électroniques quantiques Alpes (NEEL - QuantECA), and Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Nanotechnology, 02 engineering and technology, 193 nm Lithography, 010402 general chemistry, Methacrylate, Molecular weight, 01 natural sciences, law.invention, law, Resist, Electrical and Electronic Engineering, chemistry.chemical_classification, Molecular electronics, Polymer, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [ CHIM.POLY ] Chemical Sciences/Polymers, [CHIM.POLY]Chemical Sciences/Polymers, Polymer structure, chemistry, Radius of gyration, Molar mass distribution, Photo acid generator, Photolithography, 0210 nano-technology, Critical dimension
Abstract

International audience; Miniaturization in microelectronic technologies requests a development of new high-performance materials for microlithography with good resolution of the critical dimension. However, the real impact of polymer structure on lithographic performances is not yet well understood to predict the properties of formulated resist. Our approach is the synthesis and characterization of model resists and the understanding of the relationship between material - properties - processes. In this work we present the influence of the polymer's molecular weight in lithographic profile of the generated patterns. The limits of the polymer's molecular weight values based on model terpolymers, consisting of methacrylate matrix, for efficient patterning have been identified. Finally, the ineffective sensitivity and dissolution issue of the polymer resists having an average molecular weight of 30 kg/mol was extensively examined and attributed to the molecular weight of the polymer and more precisely to the radius of gyration of the polymer.

Published
2009
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14. A study of thermal decomposition and combustion products of disposable polyethylene terephthalate (PET) plastic using high resolution fourier transform infrared spectroscopy, selected ion flow tube mass spectrometry and gas chromatography mass spectrometry

Author

Kseniya Dryahina, Kristýna Sovová, Martin Ferus, I. Matulková, Otto Dvořák, Svatopluk Civiš, Patrik Španěl, J. Heyrovský Institute of Physical Chemistry, Czech Academy of Sciences [Prague] (CAS), Chemical Physics, J. Heyrovsky Institute of Physical Chemistry, and Fire Technical Institute

Subjects
Terephthalic acid, Chemistry, 010401 analytical chemistry, Xylene, Biophysics, Analytical chemistry, 02 engineering and technology, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Ethylbenzene, 0104 chemical sciences, 3. Good health, Styrene, chemistry.chemical_compound, 13. Climate action, Physical Sciences, Polyethylene terephthalate, Selected-ion flow-tube mass spectrometry, Physical and Theoretical Chemistry, Fourier transform infrared spectroscopy, 0210 nano-technology, Benzene, Molecular Biology
Abstract

International audience; The industrial production of poly (ethylene terephthalate), PET, continues to increase and thus it is important to understand the composition of fumes resulting from its disposal as a part of incinerated waste. In this study samples of PET material were combusted in a furnace corresponding to the German standard DIN 53 436 at the temperatures of 500○C, 800○C (in an air flow) and also uncontrolled burning in air. The gaseous products were then analysed using three different analytical methods: high resolution Fourier transform infrared spectroscopy (FTIR), selected ion flow tube mass spectrometry (SIFT-MS) and gas chromatography mass spectrometry (GC-MS). Carbon dioxide, methane, ethylene, acetylene, formaldehyde (methanal) and acetaldehyde (ethanal) were detected by FTIR. Water, methane, acetaldehyde, ethylene, formaldehyde, methanol, acetone, benzene, terephthalic acid, styrene (ethenylbenzene), ethanol, toluene (methylbenzene), xylene (dimethylbenzene), ethylbenzene, naphthalene, biphenyl and phenol concentrations were all quantified by both SIFT-MS and GC-MS. Additionally, the fumes resulting from uncontrolled combustion in air were analysed by FTIR which resolves the rotation-vibration structure of the absorption bands of formaldehyde (2779.90 and 2778.48 cm-1) and propane, which was identified from characteristic vibrations of CH3 groups at 2977.00 and 2962.00 cm-1. The spectra were compared to the reference standards.

Published
2008
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15. Potentiality of the 'Gum Metal' titanium-based alloy for biomedical applications

Author

D.M. Gordin, Cora Vasilescu, Anisoara Cimpean, Raluca Ion, Thierry Gloriant, Silviu Iulian Drob, 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), Department of Biochemistry and Molecular Biology, University of Bucharest (UniBuc), Institute of Physical Chemistry 'Ilie Murgulescu', Institute of Physical Chemistry, 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), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)

Subjects
Materials science, Biocompatibility, Simulated body fluid, Alloy, chemistry.chemical_element, Modulus, Bioengineering, Biocompatible Materials, 02 engineering and technology, engineering.material, 01 natural sciences, Corrosion, Biomaterials, Mice, 3T3-L1 Cells, Elastic Modulus, 0103 physical sciences, Materials Testing, Alloys, Animals, [CHIM]Chemical Sciences, Composite material, Cell Proliferation, 010302 applied physics, Titanium, Osteoblasts, Metallurgy, Gum metal, technology, industry, and agriculture, Titanium alloy, Cell Differentiation, Electrochemical Techniques, 021001 nanoscience & nanotechnology, equipment and supplies, 3. Good health, Body Fluids, chemistry, Mechanics of Materials, engineering, 0210 nano-technology
Abstract

International audience; In this study, the "Gum Metal" titanium-based alloy (Ti-23Nb-0.7Ta-2Zr-1.2O) was synthesized by melting and then characterized in order to evaluate its potential for biomedical applications. Thus, the mechanical properties, the corrosion resistance in simulated body fluid and the in vitro cell response were investigated. It was shown that this alloy presents a very high strength, a low Young's modulus and a high recoverable strain by comparison with the titanium alloys currently used in medicine. On the other hand, all electrochemical and corrosion parameters exhibited more favorable values showing a nobler behavior and negligible toxicity in comparison with the commercially pure Ti taken as reference. Furthermore, the biocompatibility tests showed that this alloy induced an excellent response of MC3T3-E1 pre-osteoblasts in terms of attachment, spreading, viability, proliferation and differentiation. Consequently, the "Gum Metal" titanium-based alloy processes useful characteristics for the manufacturing of highly biocompatible medical devices.

Published
2014
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16. Artificial Iono- and Photosensitive Membranes Based on an Amphiphilic Aza-Crown-Substituted Hemicyanine

Author

Christine Grauby-Heywang, Sophiya Selektor, Vladimir V. Arslanov, Daria A. Silant’yeva, Pinar Batat, Gediminas Jonusauskas, Nathan D. McClenaghan, Laboratoire Ondes et Matière d'Aquitaine (LOMA), Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Frumkin Institute of Physical Chemistry and Electrochemistry (RAS), Russian Academy of Sciences [Moscow] (RAS), Institut des Sciences Moléculaires (ISM), Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Centre National de la Recherche Scientifique (CNRS), Centre de physique moléculaire optique et hertzienne (CPMOH), Centre National de la Recherche Scientifique (CNRS)-Université Sciences et Technologies - Bordeaux 1, Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and A.N. Frumkin Institute of Physical Chemistry and Electrochemistry

Subjects
Dimer, 02 engineering and technology, 010402 general chemistry, Photochemistry, Excimer, 01 natural sciences, Fluorescence spectroscopy, Surface-Active Agents, chemistry.chemical_compound, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Cations, Amphiphile, Ultrafast laser spectroscopy, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Physical and Theoretical Chemistry, Coloring Agents, ComputingMilieux_MISCELLANEOUS, Langmuir-Blodgett films, [PHYS]Physics [physics], Aza Compounds, Molecular Structure, Excimers, [PHYS.PHYS]Physics [physics]/Physics [physics], Chemistry, Carbocyanines, Photochemical Processes, 021001 nanoscience & nanotechnology, Ion-sensitive membranes, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Membrane, Microscopy, Fluorescence, Absorption (chemistry), 0210 nano-technology, Hemicyanines, Fluorescence anisotropy
Abstract

International audience; Artificial iono- and photosensitive membranes based on an amphiphilic aza-crown-substituted hemicyanine are assembled on liquid and solid supports and their aggregation behaviour, which is influenced by the binding of metal cations and surface density, is studied. The photoinduced charge-transfer properties of an analogous non-amphiphilic hemicyanine in solution are also demonstrated. An asymmetric sandwich dimer model is proposed and existence of such dimers in solution is evidenced by transient absorption and fluorescence anisotropy experiments. Changes in absorption and emission spectra, as well as compression isotherms of the amphiphile observed in the presence of cations, are discussed in terms of 2D molecular reorganisation. Surface-pressure-controlled reversible excimer formation at the air-water interphase and excimer-type emission of Langmuir-Blodgett films in the presence of cations are demonstrated and are discussed on the basis of fibre-optic fluorimetry and fluorescence microscopy results.

Published
2014
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17. Design of a nitrogen-implanted titanium-based superelastic alloy with optimized properties for biomedical applications

Author

Valentina Mitran, Denis Busardo, Silviu Iulian Drob, Thierry Gloriant, Cora Vasilescu, Anisoara Cimpean, M. Cornen, Daniel Höche, D.M. Gordin, 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), Quertech Ingenierie, Department of Biochemistry and Molecular Biology, University of Bucharest (UniBuc), Institute of Physical Chemistry 'Ilie Murgulescu', Institute of Physical Chemistry, Institute of Materials Research [Geesthacht], Helmholtz-Zentrum Geesthacht (GKSS), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and 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)

Subjects
Surface analysis, Corrosion resistance, 02 engineering and technology, Nitride, 01 natural sciences, [CHIM.GENI]Chemical Sciences/Chemical engineering, X-Ray Diffraction, Composite material, Titanium, Photoelectron Spectroscopy, 021001 nanoscience & nanotechnology, Body Fluids, Corrosion, Ion implantation, Mechanics of Materials, Biocompatibility, Titanium alloy, 0210 nano-technology, Materials science, Friction, Nitrogen, Surface Properties, Alloy, Biomedical Technology, chemistry.chemical_element, Bioengineering, engineering.material, 010402 general chemistry, Biomaterials, Fetus, X-ray photoelectron spectroscopy, Hardness, Tensile Strength, Alloys, Humans, ddc:620.11, Cell Proliferation, Osteoblasts, L-Lactate Dehydrogenase, Metallurgy, technology, industry, and agriculture, Elasticity, Fibronectins, 0104 chemical sciences, chemistry, Potentiometry, engineering, Stress, Mechanical
Abstract

International audience; In this study, a superelastic Ni-free Ti-based biomedical alloy was treated in surface by the implantation of nitrogen ions for the first time. The N-implanted surface was characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and secondary ion mass spectroscopy, and the superficial mechanical properties were evaluated by nano-indentation and by ball-on-disk tribological tests. To investigate the biocompatibility, the corrosion resistance of the N-implanted Ti alloy was evaluated in simulated body fluids (SBF) complemented by in-vitro cytocompatibility tests on human fetal osteoblasts. After implantation, surface analysis methods revealed the formation of a titanium-based nitride on the substrate surface. Consequently, an increase in superficial hardness and a significant reduction of friction coefficient were observed compared to the non-implanted sample. Also, a better corrosion resistance and a significant decrease in ion release rates have been obtained. Cell culture experiments indicated that the cytocompatibility of the N-implanted Ti alloy was superior to that of the corresponding non-treated sample. Thus, this new functional N-implanted titanium-based superelastic alloy presents the optimized properties that are required for various medical devices: superelasticity, high superficial mechanical properties, high corrosion resistance and excellent cytocompatibility.

Published
2013
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18. Bimodal mesoporous titanium dioxide anatase films templated by a block polymer and an ionic liquid: influence of the porosity on the permeability

Author

Mathieu Etienne, Bernd M. Smarsly, Michael Schröder, Christian Dunkel, Sébastien Sallard, Cédric Boissière, Alain Walcarius, Torsten Oekermann, Michael Wark, Paul Scherrer Institute (PSI), Institute of physical chemistry, Justus-Liebig-Universität Gießen = Justus Liebig University (JLU), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institute of physical chemistry and electrochemistry, Leibniz Universität Hannover=Leibniz University Hannover, Laboratoire de Chimie Physique et Microbiologie pour l'Environnement (LCPME), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Carl Von Ossietzky Universität Oldenburg = Carl von Ossietzky University of Oldenburg (OFFIS), Ruhr-Universität Bochum [Bochum], Institute of Physical Chemistry, Justus-Liebig-Universität Gießen (JLU), Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC), Leibniz Universität Hannover [Hannover] (LUH), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), and Carl Von Ossietzky Universität Oldenburg

Subjects
Anatase, Materials science, silica thin-films, Chemistry & allied sciences, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, molecular-transport, chemistry.chemical_compound, generation, Copolymer, General Materials Science, crystalline, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Porosity, chemistry.chemical_classification, sensitized solar-cells, tio2 films, architectures, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, lithium batteries, accessibility, chemistry, Chemical engineering, Titanium dioxide, Ionic liquid, ddc:540, Grazing-incidence small-angle scattering, 0210 nano-technology, Mesoporous material, performance
Abstract

In the present paper, we report the synthesis of bimodal mesoporous anatase TiO2 films by the EISA (Evaporation-Induced Self-Assembly) method using sol-gel chemistry combining two porogen agents, a low molecular weight ionic template and a neutral block copolymer. The surfactant template (C(16)mimCl) generates non-oriented worm-like pores (8 to 10 nm) which connect the regularly packed ellipsoidal mesopores (15 to 20 nm diameter) formed by an amphiphilic block copolymer of the type poly(isobutylene)-b-poly(ethylene oxide) (PIB-PEO). The surfactant template can also significantly influence the size and packing of the ellipsoidal mesopores. The mesostructural organization and mesoporosity of the films are studied by Environmental Ellipsometry-Porosimetry (EEP), Grazing-Incidence Small-Angle X-ray Scattering (GISAXS) and electron microscopy techniques. Electrochemical characterization is performed to study the permeability of the films to liquid solutions, using two types of probe moieties (K3FeIII(CN)(6) and Ru(bpy)(3)(2+)) by the wall-jet technique. An optimum ratio of C(16)mimCl/PIB-PEO provides anatase films with a continuous bimodal mesopore structure, possessing a permeability up to two times higher than that of the mesoporous films templated by PIB-PEO only (with partially isolated mesopores). When C(16)mimCl is used in large quantities, up to 20% weight vs. PIB-PEO, large overall porous volume and surface area are obtained, but the mesostructure is increasingly disrupted, leading to a severe loss of permeability of the bimodal films. A dye-sensitized solar cell set-up is used with anatase films as the photoelectrode. The photosensitizer loading and the total energy conversion efficiency of the solar cells using the mesoporous films templated by an optimal ratio of the two porogen agents C(16)mimCl and PIB-PEO can be substantially increased in comparison with the solar cells using mesoporous films templated by PIB-PEO only. DFG/SM 199/6-1 DFG/OE 420/5-1 BMBF/SOHyb/03X3525E

Published
2013
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19. Surface characterization and biocompatibility of titanium alloys implanted with nitrogen by Hardion+ technology

Author

V. Chane-Pane, Valentina Mitran, Cora Vasilescu, Thierry Gloriant, Denis Busardo, Anisoara Cimpean, Daniel Höche, D.M. Gordin, Silviu Iulian Drob, 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), Quertech Ingenierie, Department of Biochemistry and Molecular Biology, University of Bucharest (UniBuc), Institute of Materials Research [Geesthacht], Helmholtz-Zentrum Geesthacht (GKSS), Institute of Physical Chemistry 'Ilie Murgulescu', Institute of Physical Chemistry, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and 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)

Subjects
Materials science, Ion beam, Biocompatibility, Cell Survival, Nitrogen, Surface Properties, Alloy, Biomedical Engineering, Biophysics, chemistry.chemical_element, Bioengineering, Biocompatible Materials, 02 engineering and technology, engineering.material, Mass Spectrometry, Corrosion, Biomaterials, 03 medical and health sciences, chemistry.chemical_compound, Materials Testing, Alloys, Cell Adhesion, Humans, 030304 developmental biology, Cell Proliferation, Ions, Titanium, 0303 health sciences, Osteoblasts, Metallurgy, technology, industry, and agriculture, Temperature, Titanium alloy, Prostheses and Implants, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, equipment and supplies, Titanium nitride, Extracellular Matrix, Fibronectins, chemistry, Chemical engineering, engineering, 0210 nano-technology, Tin
Abstract

International audience; In this study, the new Hardion+ micro-implanter technology was used to modify surface properties of biomedical pure titanium (CP-Ti) and Ti-6Al-4V ELI alloy by implantation of nitrogen ions. This process is based on the use of an electron cyclotron resonance ion source to produce a multienergetic ion beam from multicharged ions. After implantation, surface analysis methods revealed the formation of titanium nitride (TiN) on the substrate surfaces. An increase in superficial hardness and a significant reduction of friction coefficient were observed for both materials when compared to non-implanted samples. Better corrosion resistance and a significant decrease in ion release rates were observed for N-implanted biomaterials due to the formation of the protective TiN layer on their surfaces. In vitro tests performed on human fetal osteoblasts indicated that the cytocompatibility of N-implanted CP-Ti and Ti-6Al-4V alloy was enhanced in comparison to that of the corresponding non treated samples. Consequently, Hardion+ implantation technique can provide titanium alloys with better qualities in terms of corrosion resistance, cell proliferation, adhesion and viability.

Published
2012
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20. Synthesis and characterization of a new superelastic Ti-25Ta-25Nb biomedical alloy

Author

Ecaterina Vasilescu, Emmanuel Bertrand, D.M. Gordin, Paula Drob, Thierry Gloriant, Silviu Iulian Drob, Cora Vasilescu, 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), Institute of Physical Chemistry 'Ilie Murgulescu', Institute of Physical Chemistry, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and 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)

Subjects
6111 aluminium alloy, Materials science, Corrosion tests, Niobium, Alloy, Biomedical Engineering, Mechanical properties, 02 engineering and technology, Tantalum, 5005 aluminium alloy, engineering.material, 01 natural sciences, Corrosion, Biomaterials, Coated Materials, Biocompatible, Tensile Strength, 0103 physical sciences, Alloys, Elastic modulus, Microstructure, ComputingMilieux_MISCELLANEOUS, 010302 applied physics, Titanium, Metallurgy, technology, industry, and agriculture, Temperature, Titanium alloy, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Elasticity, Ringer's Solution, Mechanics of Materials, Melting point, engineering, Stress, Mechanical, Isotonic Solutions, 0210 nano-technology
Abstract

In this study, a new Ti–25Ta–25Nb (mass%) beta alloy was synthesised by cold crucible semi-levitation melting. This technique made it possible to obtain homogeneous ingots although the elements used have very different melting points. After melting, a thermo-mechanical treatment was applied in order to obtain a perfectly recrystallised beta microstructure. For this alloy composition, the tensile tests showed a very low Young’s modulus associated with an important super-elastic behaviour, which contributes to decrease the elastic modulus under stress and to increase the recoverable strain. On the other hand, the corrosion tests, which were carried out in a neutral Ringer solution, indicated a corrosion resistance higher than that of the commercially pure CP Ti alloy. These results show that this new alloy possesses all the characteristics necessary for its long-term use in medical implants.

Published
2010
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21. Accurate determination of low state rotational quantum numbers (J < 4) from planar-jet and liquid nitrogen cell absorption spectra of methane near 1.4 micron

Author

Alain Campargue, Petr Pracna, Samir Kassi, Milan Mašát, Ondřej Votava, J. Heyrovsky Institute of Physical Chemistry, J. Heyrosky´ Institute of Physical Chemistry (IPC), Czech Academy of Sciences [Prague] (CAS), J. Heyrovsky institute of Physical Chemistry, LAsers, Molécules et Environnement (LAME-LIPhy), Laboratoire Interdisciplinaire de Physique [Saint Martin d’Hères] (LIPhy), Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF), J. Heyrovsky Institute of Physical Chemistry (JH-INST), Laboratoire de Spectrométrie Physique (LSP), Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS), and ANR-08-BLAN-2-321467,ANR-08-BLAN,CH4@Titan(2008)

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Jet (fluid), [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], 010304 chemical physics, Absorption spectroscopy, Chemistry, Analytical chemistry, General Physics and Astronomy, 02 engineering and technology, Liquid nitrogen, 021001 nanoscience & nanotechnology, Quantum number, 7. Clean energy, 01 natural sciences, Spectral line, Methane, chemistry.chemical_compound, 0103 physical sciences, Supersonic speed, Physical and Theoretical Chemistry, Atomic physics, 0210 nano-technology, Spin (physics), ComputingMilieux_MISCELLANEOUS
Abstract

International audience; An improved procedure for accurate determination of empirical lower state rotational quantum numbers from molecular absorption spectra is demonstrated for methane. We combine the high resolution absorption spectra in the 7070–7300 cm−1 frequency range obtained in liquid nitrogen cooled cryogenic cell (T = 81 K) and in supersonic planar jet expansion (TR = 25 K). Empirical lower state energies of 59 transitions are determined from the ratio of the absolute absorption line strengths at 25 and 81 K. The procedure relies on the realistic description of rotational state populations in the supersonic jet expansion where non-equilibrium nuclear spin isomer distributions are generated due to the rapid cooling. The accuracy of the experimental determination of the lower state energies with J ≤ 3 is found to considerably improve the results of the same approach applied to spectra at 296 and 81 K. The 59 transitions with determined lower J values provide a good starting point for the theoretical interpretation of the highly congested icosad region of methane. In particular, the centres of nine vibrational bands are estimated from the transitions with J = 0 lower state rotational quantum number.

Published
2010
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22. Raman scattering boson peak and differential scanning calorimetry studies of the glass transition in tellurium–zinc oxide glasses

Author

S. Khatir, Athanassios G. Kontos, Bruno Capoen, M. Bouazaoui, R D Tsopouridou, C. Raptis, S. Kripotou, Sylvia Turrell, Elissaios Stavrou, C Tsiantos, Department of Physics, National Technical University of Athens, Institute of Physical Chemistry 'Demokritos' ( IPC ), National Center for Scientific Research 'Demokritos' ( NCSR ), Centre d'Etudes et de Recherches Lasers et Applications ( CERLA ), Université de Lille, Sciences et Technologies, Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 ( PhLAM ), Université de Lille-Centre National de la Recherche Scientifique ( CNRS ), Laboratoire de Spectrochimie Infrarouge et Raman - UMR 8516 ( LASIR ), National Technical University of Athens [Athens] (NTUA), Institute of Physical Chemistry 'Demokritos' (IPC), National Center for Scientific Research 'Demokritos' (NCSR), Centre d'Etudes et de Recherches Lasers et Applications (CERLA), Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 (LASIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Centrale Lille Institut (CLIL), and Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Oxide, Analytical chemistry, [ PHYS.COND.CM-MS ] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], chemistry.chemical_element, 02 engineering and technology, Zinc, Spectrum Analysis, Raman, 01 natural sciences, Phase Transition, symbols.namesake, chemistry.chemical_compound, Differential scanning calorimetry, 0103 physical sciences, General Materials Science, 010306 general physics, Calorimetry, Differential Scanning, Temperature, 021001 nanoscience & nanotechnology, Condensed Matter Physics, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [ PHYS.PHYS.PHYS-CHEM-PH ] Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], chemistry, [ CHIM.THEO ] Chemical Sciences/Theoretical and/or physical chemistry, symbols, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Boson peak, Glass, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Tellurium, Zinc Oxide, 0210 nano-technology, Glass transition, Raman spectroscopy, Raman scattering
Abstract

Raman scattering and differential scanning calorimetry (DSC) measurements have been carried out on four mixed tellurium–zinc oxide (TeO2)1 − x(ZnO)x (x = 0.1, 0.2, 0.3, 0.4) glasses under variable temperature, with particular attention being given to the respective glass transition region. From the DSC measurements, the glass transition temperature Tg has been determined for each glass, showing a monotonous decrease of Tg with increasing ZnO content. The Raman study is focused on the low-frequency band of the glasses, the so-called boson peak (BP), whose frequency undergoes an abrupt decrease at a temperature Td very close to the respective Tg values obtained by DSC. These results show that the BP is highly sensitive to dynamical effects over the glass transition and provides a means for an equally reliable (to DSC) determination of Tg in tellurite glasses and other network glasses. The discontinuous temperature dependence of the BP frequency at the glass transition, along with the absence of such a behaviour by the high-frequency Raman bands (due to local atomic vibrations), indicates that marked changes of the medium range order (MRO) occur at Tg and confirms the correlation between the BP and the MRO of glasses.

Published
2010
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23. Proton-Coupled Oxygen Reduction At Liquid-Liquid Interfaces Catalyzed By Cobalt Porphine

Author

Manuel A. Méndez, Fei Li, Mustafa Ersoz, Tony Khoury, Hubert H. Girault, Bin Su, Jean-Michel Barbe, Zdenek Samec, Claude P. Gros, Imren Hatay, Ecole Polytechnique Fédérale de Lausanne ( EPFL ), Selcuk University, Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] ( ICMUB ), Université de Bourgogne ( UB ) -Centre National de la Recherche Scientifique ( CNRS ), J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of Czech Republic, Czech Academy of Sciences [Prague] ( ASCR ), Ecole Polytechnique Fédérale de Lausanne (EPFL), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), Centre National de la Recherche Scientifique (CNRS)-Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC), Heyrovský Institute of Physical Chemistry of the Czech Academy of Sciences (HIPC / CAS), and Czech Academy of Sciences [Prague] (CAS)

Subjects
Metalloporphyrins, Inorganic chemistry, chemistry.chemical_element, Electrons, Electron donor, 02 engineering and technology, Electrolyte, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Biochemistry, Catalysis, Electron Transport, [ CHIM.CATA ] Chemical Sciences/Catalysis, Electron transfer, chemistry.chemical_compound, Scanning electrochemical microscopy, Colloid and Surface Chemistry, Electrochemistry, porphyrine, ITIES, Voltammetry, ComputingMilieux_MISCELLANEOUS, dioxygen reduction, Aqueous solution, Electric Conductivity, Water, biphasic system, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, Hydrogen-Ion Concentration, 021001 nanoscience & nanotechnology, cobalt, 0104 chemical sciences, Oxygen, Kinetics, chemistry, Thermodynamics, Protons, 0210 nano-technology, Oxidation-Reduction, Cobalt
Abstract

Cobalt porphine (CoP) dissolved in the organic phase of a biphasic system is used to catalyze O(2) reduction by an electron donor, ferrocene (Fc). Using voltammetry at the interface between two immiscible electrolyte solutions (ITIES), it is possible to drive this catalytic reduction at the interface as a function of the applied potential difference, where aqueous protons and organic electron donors combine to reduce O(2). The current signal observed corresponds to a proton-coupled electron transfer (PCET) reaction, as no current and no reaction can be observed in the absence of either the aqueous acid, CoP, Fc, or O(2).

Published
2009
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24. Streaming Potential in Cylindrical Pores of Poly(ethylene terephthalate) Track-Etched Membranes: Variation of Apparent ζ Potential with Pore Radius

Author

V. D. Sobolev, Vladimir V. Berezkin, Vitaly I. Volkov, Philippe Dejardin, Elena N. Vasina, Institut Européen des membranes (IEM), Université de Montpellier (UM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS), Department of Technical Cybernetics, Samara State University, Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM), A. V. Shubnikov Institute of Crystallography (IC RAS), Russian Academy of Sciences [Moscow] (RAS), Institute of Physical Chemistry of the RAS, and Karpov Institute of Physical Chemistry

Subjects
Ion beam, Chemistry, Mordançage, Analytical chemistry, Mineralogy, Resonance, Conductance, Ionic bonding, 02 engineering and technology, Surfaces and Interfaces, Radius, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Streaming current, 0104 chemical sciences, Membrane, Electrochemistry, [CHIM]Chemical Sciences, General Materials Science, 0210 nano-technology, Spectroscopy, ComputingMilieux_MISCELLANEOUS
Abstract

Streaming potential variation with pressure measured through poly(ethylene terephthalate) track-etched membranes of different pore sizes led to the determination of an apparent interfacial potential zetaa in the presence of 10-2 M KCl. The variation of zetaa with the pore radius r0 is interpreted by (i) the electric double layer overlap effect and (ii) the presence of a conductive gel layer. We propose a method which integrates both effects by assuming a simple model for the conductive gel at the pore wall. We observed the following three domains of pore size: (i) r0 > 70 nm, where surface effects are negligible; (ii) approximately 17 nm < r0 < 70 nm, where the pore/solution interface could be described as a conductive gel of thickness around 1 nm; (iii) r0 < approximately 17 nm, which corresponds to the region strongly damaged by the ion beam and is not analyzed here. The first one (zeta = -36.2 mV) corresponds to the raw material when etching has completely removed the ion beam predamaged region, which corresponds to the second intermediate domain (zeta = -47.3 mV). There the conductance of the gel layer deduced from the treatment of streaming potential data was found to be compatible with the number of ionic sites independently determined by the electron spin resonance technique.

Published
2005
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25. Electroactive ceramic carbon electrode modified with ionic liquid

Author

Ewa Rozniecka, Laurent Gaillon, Juliette Sirieix-Plenet, Marcin Opallo, Galyna Shul, Laboratoire d'Electrochimie et de Chimie Analytique (LECA), Université Pierre et Marie Curie - Paris 6 (UPMC)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Institute of Physical Chemistry, Institute of Physical chemistry, and Institue of Physical Chemistry

Subjects
Working electrode, Cyclic voltammetry, Standard hydrogen electrode, Inorganic chemistry, 02 engineering and technology, Ionic liquid, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Reference electrode, lcsh:Chemistry, Quinhydrone electrode, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Electrochemistry, Redox reaction, Sol-gel, Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, lcsh:Industrial electrochemistry, lcsh:QD1-999, Saturated calomel electrode, Palladium-hydrogen electrode, Carbon ceramic electrode, 0210 nano-technology, Electrode potential, lcsh:TP250-261
Abstract

The electrode based on silicate carbon composite material was modified with redox probe (t-butylferrocene) solution in ionic liquid (1-butyl-3-methylimidazolium hexafluorophosphate or 1-decyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide). After immersion into an aqueous solution it was studied by cyclic voltammetry. It exhibits electrochemical signal connected with electrode reaction of the redox probe dissolved in ionic liquid. The heterogeneous structure of electrode material enhances substantially efficiency of the electrode process in comparison to the drop deposited on flat electrode surface. The midpeak potential depends on the hydrophobicity of the anion present in the aqueous solution indicating significant contribution of anion injection into the ionic liquid following the electron transfer. The efficiency of the electrode process is much larger than that of similar electrode modified with the redox probe solution in less viscous organic polar solvent. Keywords: Carbon ceramic electrode, Ionic liquid, Redox reaction, Sol–gel, Cyclic voltammetry

Published
2005
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26. Observation of negative line tensions from Plateau border regions in dry foam films

Author

F. Caillier, J.-C. Géminard, Patrick Oswald, A. Żywocinski, École normale supérieure - Lyon (ENS Lyon), Institute of Physical Chemistry, Institute of Physical Chemistry Polish Academy of Sciences, and École normale supérieure de Lyon (ENS de Lyon)

Subjects
Materials science, Ccd camera, Mineralogy, 02 engineering and technology, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Plateau (mathematics), 01 natural sciences, [PHYS.PHYS.PHYS-GEN-PH]Physics [physics]/Physics [physics]/General Physics [physics.gen-ph], Tension (geology), 0103 physical sciences, Soap film, Composite material, 010306 general physics, 0210 nano-technology, Line (formation)
Abstract

International audience; We measure the angles produced in the Plateau border region of " dry " soap films. In a simple experimental geometry, we demonstrate that a negative line tension can be attributed to these regions. This result has important consequences for the theoretical description of foams approaching the dry limit.

Published
2004
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27. Environmental Control of Single‐Molecule Junction Evolution and Conductance: A Case Study of Expanded Pyridinium Wiring

Author

Gábor Mészáros, Philippe P. Lainé, Jakub Šebera, Viliam Kolivoška, Štěpánka Nováková Lachmanová, Magdaléna Hromadová, Jindřich Gasior, Grégory Dupeyre, J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Division of Livestock Sciences, Universität für Bodenkultur Wien [Vienne, Autriche] (BOKU), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)

Subjects
expanded pyridiniums, Materials science, 02 engineering and technology, Substrate (electronics), 010402 general chemistry, 01 natural sciences, Catalysis, law.invention, chemistry.chemical_compound, law, Water environment, [CHIM]Chemical Sciences, Molecule, ComputingMilieux_MISCELLANEOUS, Research Articles, 010405 organic chemistry, Conductance, Molecular electronics, General Medicine, General Chemistry, 021001 nanoscience & nanotechnology, solvent gating, 0104 chemical sciences, chemistry, Chemical physics, single-molecule conductance, scanning tunneling microscopy, Pyridinium, Molecular Electronics, Scanning tunneling microscope, 0210 nano-technology, Break junction, Research Article
Abstract

Environmental control of single‐molecule junction evolution and conductance was demonstrated for expanded pyridinium molecules by scanning tunneling microscopy break junction method and interpreted by quantum transport calculations including solvent molecules explicitly. Fully extended and highly conducting molecular junctions prevail in water environment as opposed to short and less conducting junctions formed in non‐solvating mesitylene. A theoretical approach correctly models single‐molecule conductance values considering the experimental junction length. Most pronounced difference in the molecular junction formation and conductance was identified for a molecule with the highest stabilization energy on the gold substrate confirming the importance of molecule–electrode interactions. Presented concept of tuning conductance through molecule–electrode interactions in the solvent‐driven junctions can be used in the development of new molecular electronic devices., Single‐molecule junction conductance can be efficiently tuned by solvent environment. A series of expanded pyridinium molecular wires gave higher conductance with fully extended junction geometries in solvating water environment as opposed to mesitylene solvent. Environmental control efficiently operates the molecule–electrode interactions.

Published
2021
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28. Solvothermal and mechanochemical intercalation of Cu into La2O2S2 enabled by the redox reactivity of (S2)2− pairs

Author

Catherine Guillot-Deudon, Gwladys Steciuk, Etienne Janod, Isabelle Braems, Laurent Cario, Stéphane Jobic, Benoit Corraze, Shunsuke Sasaki, Maria Teresa Caldes, Institut des Matériaux Jean Rouxel (IMN), 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)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), J. Heyrovský Institute of Physical Chemistry of the ASCR, and Czech Academy of Sciences [Prague] (CAS)

Subjects
Materials science, Intercalation (chemistry), 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Redox, 0104 chemical sciences, Inorganic Chemistry, Metal, visual_art, Polymer chemistry, visual_art.visual_art_medium, Reactivity (chemistry), 0210 nano-technology, Ball mill
Abstract

International audience; Intercalation of Cu into layered polychalcogenide La2O2S2 was demonstrated to be viable both in solvothermal condition at 200 °C and mechanical ball milling at ambient temperature. This result evidences the soft-chemical nature of metal intercalation into layered polychalcogenides driven by redox reactivity of anionanion bonds.

Published
2021
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29. Strain and Piezo-Doping Mismatch between Graphene Layers

Author

Martin Kalbac, Denis Machon, Alfonso San-Miguel, Félix Balima, Rémy Fulcrand, Alexis Forestier, G.S. Pinheiro, Colin Bousige, Spectroscopies optiques des matériaux verres, amorphes et à nanoparticules (SOPRANO), Institut Lumière Matière [Villeurbanne] (ILM), 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-Centre National de la Recherche Scientifique (CNRS), Luminescence (LUMINESCENCE), Laboratoire des Multimatériaux et Interfaces (LMI), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), (nano)Matériaux pour l'énergie (ENERGIE), Departamento de Física, Campus Ministro Petrônio Portella Bloco 03, Universidade Federal do Piauí, Universidade Federal do Piauí, Liquides et interfaces (L&I), J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Laboratoire Nanotechnologies et Nanosystèmes [Sherbrooke] (LN2), Université de Sherbrooke (UdeS)-École Centrale de Lyon (ECL), Université de Lyon-Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE)-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)-Université Grenoble Alpes (UGA), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon

Subjects
Materials science, Nitrogen, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Two dimensional materials, law, Doping, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Physical and Theoretical Chemistry, Electronic properties, [PHYS]Physics [physics], Strain (chemistry), business.industry, Graphene, Bilayer, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, Modulation, Alcohols, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optoelectronics, Layers, 0210 nano-technology, business
Abstract

International audience; Modulation of electronic properties of bilayer materials through the strain and doping mismatch between layers opens new opportunities in 2D material straintronics. We present here a new approach allowing to generate asymmetric strain or doping between layers and a method to quantify it using a supported isotopically labeled bilayer graphene studied by in situ Raman spectroscopy. Strain differences up to ∼0.1% between the two graphene layers have been obtained by applying pressures of up to 10 GPa with nonpolar solid environments. However, when immersed in a liquid polar environment, namely, a mixture of ethanol and methanol, a piezo-doping mismatch between layers is observed. This asymmetrical doping increases with pressure, leading to charge concentration differences between layers of the order of 1013 cm–2. Our approach thus allows disentangling strain and doping effects in high-pressure experiments evidencing the asymmetries of these phenomena and comforting isotopic bilayer graphene as a benchmark system for the study of asymmetric effects in devices or composite surfaces.

Published
2020
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30. High-Throughput Experimentation and Computational Freeway Lanes for Accelerated Battery Electrolyte and Interface Development Research

Author

Anass Benayad, Fuzhan Rahmanian, Diddo Diddens, Martin Winter, Christian Wölke, Yuyoung Shin, Peng Yan, Helge S. Stein, Andreas Heuer, Frédéric Le Cras, Anand Narayanan Krishnamoorthy, Maxime Legallais, Isidora Cekic-Laskovic, Moumita Maiti, Département des Technologies des NanoMatériaux (DTNM), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Forschungszentrum Jülich GmbH | Centre de recherche de Juliers, Helmholtz-Gemeinschaft = Helmholtz Association, Institute of Physical Chemistry & MEET Battery Research Centre, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Helmholtz Institute Ulm (HIU), European Project: 957189,BIG-MAP, European Project: 957213,BATTERY 2030PLUS, Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de L'Energie Solaire (INES), and Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)

Subjects
Materials science, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Renewable Energy, Sustainability and the Environment, business.industry, Interface (computing), Chemistry & allied sciences, Battery electrolyte, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Electrolyte, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, [INFO.INFO-MO]Computer Science [cs]/Modeling and Simulation, 01 natural sciences, 0104 chemical sciences, ddc:050, Development (topology), ddc:540, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Materials Science, 0210 nano-technology, Process engineering, business, Throughput (business)
Abstract

International audience; The timely arrival of novel materials plays a simultaneous key and critical role in bringing advances to our society as the pace at which major technological breakthroughs take place is usually dictated by the discovery rate at which novel materials are identified within the chemical space. High throughput experimentation and computation strategy, now widely considered as a watershed in accelerating the discovery and optimization of novel materials in virtually every field, enables simultaneous screening, synthesis and characterization of large arrays of different material classes towards identification of the lead candidates for given system and targeted application. However, the ability to acquire data, through the continued advancement of automation platforms and workflows especially in the field of battery research and development, often outpaces the ability to optimally leverage obtained data for improved decision making. Closing this gap inevitably calls for adapted algorithms, development of reliable predictive models and enhanced integration with machine learning (ML), deep learning (DL) and artificial intelligence (AI). This Review aims to highlight state-of-the-art achievements along with an assessment of current and future challenges as well as resulting perspectives towards accelerated development of advanced battery electrolytes and their interfaces.

Published
2022
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31. A Luminescent, Water-Soluble Ir(III) Complex as a Potential Photosensitizer for Two-Photon Photodynamic Therapy

Author

Elisabeta I. Szerb, Sharmistha Chatterjee, Massimo La Deda, Giovanna Palermo, Lucie Sancey, Giuseppe Strangi, Loredana Ricciardi, Institute of Physical Chemistry 'Ilie Murgulescu' Romanian Academy (ICF), Università della Calabria [Arcavacata di Rende] (Unical), CNR Istituto di Nanotecnologia (NANOTEC), Consiglio Nazionale delle Ricerche [Roma] (CNR), Institute for Advanced Biosciences / Institut pour l'Avancée des Biosciences (Grenoble) (IAB), Centre Hospitalier Universitaire [Grenoble] (CHU)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Etablissement français du sang - Auvergne-Rhône-Alpes (EFS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Case Western Reserve University [Cleveland], Sancey, Lucie, CNR-NANOTEC, Licryl-UOS Cosenza & CEMIF.Cal [Cosenza, Italy] (Department of Physics), and University of Calabria [Cosenza, Italy]

Subjects
Technology, time-resolved luminescence spectroscopy, QH301-705.5, [CHIM.THER] Chemical Sciences/Medicinal Chemistry, QC1-999, 02 engineering and technology, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 010402 general chemistry, 01 natural sciences, two-photon photodynamic therapy, cyclometalated Ir(III) complexes, [CHIM]Chemical Sciences, General Materials Science, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Biology (General), Instrumentation, QD1-999, Fluid Flow and Transfer Processes, Process Chemistry and Technology, Physics, General Engineering, [SDV.SP]Life Sciences [q-bio]/Pharmaceutical sciences, [CHIM.COOR] Chemical Sciences/Coordination chemistry, 021001 nanoscience & nanotechnology, Engineering (General). Civil engineering (General), 0104 chemical sciences, Computer Science Applications, [SDV.SP] Life Sciences [q-bio]/Pharmaceutical sciences, Chemistry, TA1-2040, 0210 nano-technology
Abstract

This work reports the study of two-photon induced properties of a highly luminescent cyclometalated Ir(III) complex, [Ir(ppy)2(en)] OOCCH3 (1), ppy = 2-phenylpyridine, en = ethylenediamine. Steady-state and time-resolved fluorescence measurements were performed by exciting 1 at the biologically relevant wavelength of 800 nm, whereas, the generation of singlet oxygen (1O2) was evaluated using 9,10-Anthracenediyl-bis(methylene)dimalonic acid (ABDA) as a detection probe. Preliminary in vitro experiments with U87-MG cells were performed, showing the potential of this compound as a two-photon photodynamic therapy (2P-PDT) agent at NIR wavelengths.

Published
2021
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32. Molecularly imprinted polymer nanoparticles-based electrochemical chemosensors for selective determination of cilostazol and its pharmacologically active primary metabolite in human plasma

Author

Franck Merlier, Piyush Sindhu Sharma, Krzysztof Noworyta, Teresa Żołek, Carlo Gonzato, Karsten Haupt, Andrzej Kutner, Wlodzimierz Kutner, Jyoti, Dorota Maciejewska, Institute of Physical Chemistry [Warsaw], Polish Academy of Sciences, Department III, Génie Enzymatique et Cellulaire (GEC), and Université de Technologie de Compiègne (UTC)-Université de Picardie Jules Verne (UPJV)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[SDV]Life Sciences [q-bio], Biomedical Engineering, Biophysics, 02 engineering and technology, Biosensing Techniques, 01 natural sciences, Molecular Imprinting, Molecularly Imprinted Polymers, Limit of Detection, Electrochemistry, Molecule, Humans, Freundlich equation, Electrodes, ComputingMilieux_MISCELLANEOUS, Detection limit, Chemistry, 010401 analytical chemistry, Molecularly imprinted polymer, Sorption, General Medicine, Electrochemical Techniques, 021001 nanoscience & nanotechnology, Combinatorial chemistry, 0104 chemical sciences, Dielectric spectroscopy, Cilostazol, [CHIM.POLY]Chemical Sciences/Polymers, Pharmaceutical Preparations, Nanoparticles, Differential pulse voltammetry, 0210 nano-technology, Selectivity, Biotechnology
Abstract

Molecularly imprinted polymer (MIP) nanoparticles-based differential pulse voltammetry (DPV) and electrochemical impedance spectroscopy (EIS) chemosensors for antiplatelet drug substance, cilostazol (CIL), and its pharmacologically active primary metabolite, 3,4-dehydrocilostazol (dhCIL), selective determination in human plasma were devised, prepared, and tested. Molecular mechanics (MM), molecular dynamics (MD), and density functional theory (DFT) simulations provided the optimum structure and predicted the stability of the pre-polymerization complex of the CIL template with the chosen functional acrylic monomers. Moreover, they accounted for the MIP selectivity manifested by the molecularly imprinted cavity with the CIL molecule complex stability higher than that for each interference. On this basis, a fast and reliable method for determining both compounds was developed to meet an essential requirement concerning the personalized drug dosage adjustment. The limit of detection (LOD) at the signal-to-noise ratio of S/N = 3 in DPV and EIS determinations using the ferrocene redox probe in a “gate effect” mode was 93.5 (±2.2) and 86.5 (±4.6) nM CIL, respectively, and the linear dynamic concentration range extended from 134 nM to 2.58 μM in both techniques. The chemosensor was highly selective to common biological interferences, including cholesterol and glucose, and less selective to structurally similar dehydroaripiprazole. Advantageously, it responded to dhCIL, thus allowing for the determination of CIL and dhCIL together. The EIS chemosensor appeared slightly superior to the DPV chemosensor concerning its selectivity to interferences. The CIL DPV sorption data were fitted with Langmuir, Freundlich, and Langmuir-Freundlich isotherms. The determined sorption parameters indicated that the imprinted cavities were relatively homogeneous and efficiently interacted with the CIL molecule.

Published
2021
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33. Fluorocarbon Vapors Slow Down Coalescence in Foams

Author

Martin Hamann, Sébastien Andrieux, Katja Steck, Pierre Muller, Cosima Stubenrauch, Patrick Kékicheff, Wiebke Drenckhan, Institut Charles Sadron (ICS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-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)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-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), Institute of Physical Chemistry, University of Stuttgart, Institut d’Etudes Avancées de l’Université de Strasbourg (USIAS), Université de Strasbourg (UNISTRA), Muller, Pierre, 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), Universität Stuttgart [Stuttgart], and Institut d’Etudes Avancées de l’Université de Strasbourg - Institute for Advanced Study (USIAS)

Subjects
Materials science, Mechanical Engineering, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, [PHYS.COND.CM-SCM] Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], Chemical engineering, Mechanics of Materials, Fluorocarbon, Coalescence (chemistry), 0210 nano-technology, [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021
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34. ZnO Nanoplatelets with Controlled Thickness: Atomic Insight into Facet‐Specific Bimodal Ligand Binding Using DNP NMR

Author

Hanako Okuno, Janusz Lewiński, Michał Terlecki, Michał Leszczyński, Małgorzata Wolska-Pietkiewicz, Gaël De Paëpe, Stanislaw Gierlotka, Saumya Badoni, Iwona Justyniak, Daniel Lee, Faculty of Chemistry, Warsaw University of Technology, Faculty of Chemistry, Magnetic Resonance (RM ), 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 (UGA)-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), Warsaw University of Technology [Warsaw], Institute of Physical Chemistry, Polish Academy of Sciences, and Laboratoire d'Etude des Matériaux par Microscopie Avancée (LEMMA )

Subjects
Facet (geometry), Materials science, chemistry.chemical_element, 02 engineering and technology, Zinc, Nuclear magnetic resonance spectroscopy, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Biomaterials, Crystallography, chemistry, Electrochemistry, [CHIM]Chemical Sciences, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021
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35. Design of metastable oxychalcogenide phases by topochemical (de)intercalation of sulfur in La2O2S2

Author

Shunsuke Sasaki, Benoit Corraze, Laurent Cario, Eric Gautron, Gwladys Steciuk, Catherine Guillot-Deudon, Etienne Janod, Maria Teresa Caldes, Lukáš Palatinus, Isabelle Braems, Gilles Frapper, Stéphane Jobic, Institut des Matériaux Jean Rouxel (IMN), 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)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), and Université de Poitiers-Institut national des sciences de l'Univers (INSU - CNRS)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Solid-state chemistry, Materials science, Chalcogenide, Science, Intercalation (chemistry), General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, General Biochemistry, Genetics and Molecular Biology, Soft chemistry, Chalcogen, chemistry.chemical_compound, Metastability, Lamellar structure, Multidisciplinary, General Chemistry, 021001 nanoscience & nanotechnology, Sulfur, 0104 chemical sciences, Crystallography, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0210 nano-technology
Abstract

Designing and synthesising new metastable compounds is a major challenge of today’s material science. While exploration of metastable oxides has seen decades-long advancement thanks to the topochemical deintercalation of oxygen as recently spotlighted with the discovery of nickelate superconductor, such unique synthetic pathway has not yet been found for chalcogenide compounds. Here we combine an original soft chemistry approach, structure prediction calculations and advanced electron microscopy techniques to demonstrate the topochemical deintercalation/reintercalation of sulfur in a layered oxychalcogenide leading to the design of novel metastable phases. We demonstrate that La2O2S2 may react with monovalent metals to produce sulfur-deintercalated metastable phases La2O2S1.5 and oA-La2O2S whose lamellar structures were predicted thanks to an evolutionary structure-prediction algorithm. This study paves the way to unexplored topochemistry of mobile chalcogen anions. Great progress has been made in topochemistry of mobile oxygen anions, but metastable compounds have not yet been achieved by deintercalation of sulfur anions. Here, the authors prepare metastable oxychalcogenide phases by taking advantage of redox-reactive sulfur dimers embedded in a layered oxysulfide.

Published
2021
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36. Evidence of tetraphenylporphyrin monoacids by ion-transfer voltammetry at polarized liquid|liquid interfaces

Author

Raheleh Partovi-Nia, Hubert H. Girault, Zdenek Samec, Jean-Michel Barbe, Claude P. Gros, Bin Su, Fei Li, Ecole Polytechnique Fédérale de Lausanne ( EPFL ), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] ( ICMUB ), Université de Bourgogne ( UB ) -Centre National de la Recherche Scientifique ( CNRS ), J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of Czech Republic, Czech Academy of Sciences [Prague] ( ASCR ), Ecole Polytechnique Fédérale de Lausanne (EPFL), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), Centre National de la Recherche Scientifique (CNRS)-Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC), Heyrovský Institute of Physical Chemistry of the Czech Academy of Sciences (HIPC / CAS), and Czech Academy of Sciences [Prague] (CAS)

Subjects
Analytical chemistry, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, chemistry.chemical_compound, [ CHIM.OTHE ] Chemical Sciences/Other, Tetraphenylporphyrin, Materials Chemistry, Liquid liquid, liquid-liquid interface, ion-transfer voltammetry, Voltammetry, ComputingMilieux_MISCELLANEOUS, Metals and Alloys, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, chemistry, Ceramics and Composites, Ion transfer, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology, porphyrin
Abstract

We present a simple methodology to illustrate the existence of tetraphenylporphyrin monoacid based on ion-transfer voltammetry at a polarized water|1,2-dichloroethane interface and organic pK values are also estimated.

Published
2008
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37. Ethane oxydehydrogenation over TiP2O7-supported NiO catalysts

Author

Ştefan-Bogdan Ivan, Florica Papa, Ioana Fechete, Ioan-Cezar Marcu, Laboratoire des Systèmes Mécaniques et d'Ingénierie Simultanée (LASMIS), Université de Technologie de Troyes (UTT), Institute of Physical Chemistry, Romanian Academy of Sciences, and University of Bucharest (UniBuc)

Subjects
Materials science, Ethylene, Non-blocking I/O, chemistry.chemical_element, 02 engineering and technology, General Chemistry, Atmospheric temperature range, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Catalysis, 0104 chemical sciences, law.invention, chemistry.chemical_compound, Nickel, [SPI]Engineering Sciences [physics], chemistry, Chemical engineering, law, Calcination, Particle size, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Titanium
Abstract

Titanium pyrophosphate-supported NiO catalysts with different Ni loadings in the range from 10 to 26 wt. % were prepared by wet impregnation, characterized by nitrogen adsorption at −196 °C, ICP-OES, XRD, CO2-TPD and H2-TPR techniques and tested in ethane oxydehydrogenation (ODH) in the temperature range from 350 to 450 °C. With increasing the Ni loading, the surface area of the catalysts decreased while the NiO particle size, the basicity and the reducibility increased strongly influencing their catalytic performance. Increasing the Ni loading boosted ethane conversion that reached 36 and 50 % at 425 and 450 °C, respectively, for the highest nickel loading catalyst. Ethylene was the main reaction product for all the catalysts. The ethylene selectivity at isoconversion increases with increasing the Ni loading. The stability of the catalysts was studied at a temperature as high as their calcination temperature, i.e. 450 °C, and at lower temperature.

Published
2021
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38. Azacalixphyrins as an Innovative Alternative for the Free-Radical Photopolymerization under Visible and NIR Irradiation without the Need of Co-Initiators

Author

Davy-Louis Versace, Olivier Siri, Vlasta Brezová, Louise Breloy, Simon Pascal, Rana Mhanna, Denis Jacquemin, Jean-Pierre Malval, 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), Institut de Science des Matériaux de Mulhouse (IS2M), Centre National de la Recherche Scientifique (CNRS)-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)-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), Institute of Physical Chemistry and Chemical Physics, Slovak University of Technology in Bratislava, 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), Centre Interdisciplinaire de Nanoscience de Marseille (CINaM), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-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)-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), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Pascal, Simon, and Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE)

Subjects
[CHIM.POLY] Chemical Sciences/Polymers, Materials science, Radical, 02 engineering and technology, 010402 general chemistry, Photochemistry, 01 natural sciences, Catalysis, law.invention, chemistry.chemical_compound, law, Materials Chemistry, Irradiation, Absorption (electromagnetic radiation), Acrylate, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Metals and Alloys, General Chemistry, 021001 nanoscience & nanotechnology, [CHIM.ORGA] Chemical Sciences/Organic chemistry, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, Photopolymer, Monomer, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Ceramics and Composites, 0210 nano-technology, Photoinitiator, Light-emitting diode
Abstract

International audience; Azacalixphyrins are unique aromatic macrocycles featuring strong absorption from the visible to the near-infrared (NIR) spectral ranges. This work demonstrates through EPR spin-trapping experiments that the N-alkyl tetrasubstituted azacalixphyrin (ACP) can lead to the formation of carbon-centered radicals initiating for the free-radical photopolymerization (FRP) of bio-based acrylate monomer upon the irradiation of several light emitting diodes, which emissions range from 455 to 660 nm. Compared to other previously reported systems, the tremendous advantage of the ACP photoinitiating system is its ability to promote photopolymerization on its own, avoiding the introduction of co-initiators. A new potential application of this promising photoinitiator is highlighted through the fabrication of well-defined microstructures under NIR laser diode irradiation at λ = 800 nm.

Published
2021
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39. The structure of polyelectrolyte complex coacervates and multilayers

Author

A. V. Subbotin, Alexander N. Semenov, Semenov, Alexander, A.V. Topchiev Institute of Petrochemical Synthesis (TIPS), Russian Academy of Sciences [Moscow] (RAS), A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Institut Charles Sadron (ICS), 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), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-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)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-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)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.POLY] Chemical Sciences/Polymers, Coacervate, Materials science, Polymers and Plastics, Organic Chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Polyelectrolyte, 0104 chemical sciences, Inorganic Chemistry, Solvent, [CHIM.POLY]Chemical Sciences/Polymers, Chemical engineering, Homogeneous, Materials Chemistry, 0210 nano-technology
Abstract

International audience; The equilibrium structure of the polyelectrolyte (PE) complex coacervates and homogeneous multilayers formed by polycations and polyanions with incompatible backbones in a poor solvent is studied using a mean-field approach. The state diagrams involving symmetric and asymmetric homogeneous phases are obtained in terms of interaction parameters, ionic strength, and composition. It is found that interfacial tension between two coexisting uniform PE phases vanishes at a certain line, where both phases remain stable and (unlike the classical critical behavior) highly distinct in composition and charge. It is also shown that a microdomain structure of the coacervate phase gets thermodynamically stable at low enough salinity. Lamellar structures arising in symmetric coacervates are investigated in all segregation regimes (weak, strong, and intermediate). The mechanism of an exponential growth of uniform multilayer thickness upon layer-by-layer deposition is elucidated. It is predicted that the exponential growth rate increases with the solution ionic strength in agreement with experimental data.

Published
2021
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40. Cell Type-Dependent Integrin Distribution in Adhesion and Migration Responses on Protein-Coated Microgrooved Substrates

Author

Ralf Kemkemer, Karen Ende, Adriana R. Kyvik, Judith Guasch, Jennifer Diemer, Adria Sales, Jaume Veciana, Imma Ratera, Joachim P. Spatz, Laboratoire des matériaux et du génie physique (LMGP ), Institut National Polytechnique de Grenoble (INPG)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Ciència de Materials de Barcelona (ICMAB), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), University of Heidelberg - Institute for Physical Chemistry, and Universität Heidelberg [Heidelberg]

Subjects
Cell type, General Chemical Engineering, Integrin, education, 02 engineering and technology, complex mixtures, Extracellular matrix, lcsh:Chemistry, 03 medical and health sciences, Distribution (pharmacology), Lack of knowledge, ComputingMilieux_MISCELLANEOUS, 030304 developmental biology, 0303 health sciences, biology, Chemistry, General Chemistry, Adhesion, [CHIM.MATE]Chemical Sciences/Material chemistry, equipment and supplies, 021001 nanoscience & nanotechnology, Cell biology, lcsh:QD1-999, biology.protein, bacteria, 0210 nano-technology
Abstract

Although integrins are responsible for the interaction of cells with their environment, e.g., the extracellular matrix or artificial substrates, there is still a lack of knowledge about their role in cell adhesion and migration on protein-coated substrates with microtopography. Understanding such interactions could lead to new applications in e.g., medical implants as well as shed light on processes such as embryonic development, angiogenesis, wound healing, and tumor progression. In this work, the influence of surface topography and chemistry on αvβ3 and α5β1 integrin-mediated cell adhesion and migration of healthy and malignant human cell types (human coronary artery endothelial cells, human osteosarcoma cells, and human skin fibroblasts cells) was studied, using microgrooved and flat substrates covered by two different extracellular proteins, fibronectin and vitronectin. Although some general behaviors can be observed, cell migration (speed, directionality, and persistence time) and morphological adaptation (cell area, aspect ratio, and circularity) of cells on protein-coated microgrooved substrates are mainly dependent on the cell type and its specific integrin expression.

Published
2019
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41. Local Structure and Dynamics in Methylammonium, Formamidinium, and Cesium Tin(II) Mixed-Halide Perovskites from 119 Sn Solid-State NMR

Author

Daniel Prochowicz, Clare P. Grey, Dominik J. Kubicki, Lyndon Emsley, Aydar Rakhmatullin, Samuel D. Stranks, Elodie Salager, Cavendish Laboratory, University of Cambridge [UK] (CAM), Institute of Physical Chemistry of the Polish Academy of Sciences, Polish Academy of Sciences (PAN), Conditions Extrêmes et Matériaux : Haute Température et Irradiation (CEMHTI), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université d'Orléans (UO), Department of Chemistry [Cambridge, UK], Laboratory of Magnetic Resonance, Ecole Polytechnique Fédérale de Lausanne (EPFL)- Institute of Chemical Sciences and Engineering, and Department of Chemical Engineering - University of Cambridge

Subjects
Anions, Halide, chemistry.chemical_element, Inorganic compounds, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, Catalysis, Ion, Degradation, Colloid and Surface Chemistry, Halogens, [CHIM]Chemical Sciences, Perovskites, Chemistry, Chemical shift, Spin–lattice relaxation, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Formamidinium, Solid-state nuclear magnetic resonance, Halogen, Physical chemistry, 0210 nano-technology, Tin
Abstract

Submitted version after revision; International audience; Organic−inorganic tin(II) halide perovskites have emerged as promising alternatives to lead halide perovskites in optoelectronic applications. While they suffer from considerably poorer performance and stability in comparison to their lead analogues, their performance improvements have so far largely been driven by trial and error efforts due to a critical lack of methods to probe their atomic-level microstructure. Here, we identify the challenges and devise a 119 Sn solid-state NMR protocol for the determination of the local structure of mixed-cation and mixed-halide tin(II) halide perovskites as well as their degradation products and related phases. We establish that the longitudinal relaxation of 119 Sn can span 6 orders of magnitude in this class of compounds, which makes judicious choice of experimental NMR parameters essential for the reliable detection of various phases. We show that Cl/Br and I/Br mixed-halide perovskites form solid alloys in any ratio, while only limited mixing is possible for I/Cl compositions. We elucidate the degradation pathways of Cs-, MA-, and FA-based tin(II) halides and show that degradation leads to highly disordered, qualitatively similar products, regardless of the A-site cation and halide. We detect the presence of metallic tin among the degradation products, which we suggest could contribute to the previously reported high conductivities in tin(II) halide perovskites. 119 Sn NMR chemical shifts are a sensitive probe of the halide coordination environment as well as of the A-site cation composition. Finally, we use variable-temperature multifield relaxation measurements to quantify ion dynamics in MASnBr 3 and establish activation energies for motion and show that this motion leads to spontaneous halide homogenization at room temperature whenever two different pure-halide perovskites are put in physical contact. ■ INTRODUCTION Organic−inorganic halide perovskites (OIHPs) have emerged as a new class of materials for solar cells and light emission applications owing to the ease of solution processing, immunity to most defects, and long charge carrier lifetimes, which can be tuned by compositional engineering. 1,2 Following the first report of perovskite-based solar cells (PSC) a decade ago, 3 the field of perovskite-based photovoltaics has been developing at a very fast pace, now reaching power conversion efficiencies of over 25%. 1,4,5 OIHPs are represented by the generic ABX 3 formula, in which A is typically a small cation such as methylammonium (CH 3 NH 3 + , MA), formamidinium (CH 3 (NH 2) 2 + , FA), and/or cesium ions. The inorganic sublattice is composed of [BX 6 ] 4− octahedra, where B is a divalent metal such as Pb 2+ , Sn 2+ , and Ge 2+ or a mixture of monovalent and trivalent metals (e.g., Ag + and In 3+) and X is a halide: I − , Br − , or Cl −. Lead halide

Published
2020
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42. Colloidal samarium oxide nanoparticles prepared by femtosecond laser ablation and fragmentation for nuclear nanomedicine

Author

Anton A. Popov, G. V. Tikhonowski, Andrei V. Kabashin, Elena A. Popova-Kuznetsova, Vladimir Duflot, Irina N. Zavestovskaya, S. M. Deyev, S. M. Klimentov, Paras N. Prasad, The National Research Nuclear University MEPhI (Moscow Engineering Physics Institute) [Moscow, Russia], Karpov Institute of Physical Chemistry, Shemyakin-Ovchinnikov Institute of Bioorganic Chemistry (IBCh RAS), Russian Academy of Sciences [Moscow] (RAS), P. N. Lebedev Physical Institute of the Russian Academy of Sciences [Moscow] (LPI RAS), University at Buffalo [SUNY] (SUNY Buffalo), State University of New York (SUNY), Laboratoire Lasers, Plasmas et Procédés photoniques (LP3), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), and Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
inorganic chemicals, Materials science, [SDV]Life Sciences [q-bio], education, Nanoparticle, Nanotechnology, 02 engineering and technology, 01 natural sciences, law.invention, 010309 optics, [SPI]Engineering Sciences [physics], Colloid, Fragmentation (mass spectrometry), law, 0103 physical sciences, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS, Laser ablation, technology, industry, and agriculture, respiratory system, 021001 nanoscience & nanotechnology, Laser, 3. Good health, Neutron capture, Femtosecond, Nanomedicine, 0210 nano-technology
Abstract

Nanotechnology promises a major improvement of efficacy of nuclear medicine by targeted delivery of radioactive agents to tumors, but this approach still needs novel efficient nanoformulations to maximize diagnostic and therapeutic functions. Here, we present a two-step method of laser ablation and fragmentation in water to produce non-radioactive 152Sm-enriched samarium oxide nanoparticles (Sm NPs), which can be converted to radioactive form of 153Sm beta-emitters by neutron capture reaction. We found that laser ablation in deionized water leads to the formation of NPs having diverse morphology and broad size dispersion. To improve size characteristics of formed NPs, we applied additional femtosecond laser fragmentation step, which made possible a good control of mean NPs size under a drastic narrowing of size dispersion, and the spherical shape of formed NPs. Obtained colloidal solutions of Sm NPs were stable for several weeks after the synthesis. The formed NPs present a very promising object for nuclear nanomedicine.

Published
2020
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43. Synthesis of High Surface Area α-K y MnO 2 Nanoneedles Using Extract of Broccoli as Bioactive Reducing Agent and Application in Lithium Battery

Author

Hanaa M. Abuzeid, Ahmed M. Hashem, Martin Winter, Christian M. Julien, Jie Li, National Research Centre - NRC (EGYPT), Institute of Physical Chemistry & MEET Battery Research Centre, School of Computer Science [Wuhan], Wuhan University [China], Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), and Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Thermogravimetric analysis, cathode, Materials science, Nanostructure, Reducing agent, lithium-ion batteries, 02 engineering and technology, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, lcsh:Technology, law.invention, law, Α-K, [CHIM]Chemical Sciences, General Materials Science, α-K y MnO 2, lcsh:Microscopy, α-KyMnO2, lcsh:QC120-168.85, MnO, lcsh:QH201-278.5, lcsh:T, green synthesis, food and beverages, 021001 nanoscience & nanotechnology, Cathode, Lithium battery, 0104 chemical sciences, α-kymno2, Chemical engineering, lcsh:TA1-2040, lcsh:Descriptive and experimental mechanics, nanoneedles, Crystallite, lcsh:Electrical engineering. Electronics. Nuclear engineering, 0210 nano-technology, lcsh:Engineering (General). Civil engineering (General), lcsh:TK1-9971, Faraday efficiency
Abstract

With the aim to reduce the entire cost of lithium-ion batteries and to diminish the environmental impact, the extract of broccoli is used as a strong benign reducing agent for potassium permanganate to synthesize &alpha, KyMnO2 cathode material with pure nanostructured phase. Material purity is confirmed by X-ray powder diffraction and thermogravimetric analyses. Images of transmission electron microscopy show samples with a spider-net shape consisting of very fine interconnected nanoneedles. The nanostructure is characterized by crystallite of 4.4 nm in diameter and large surface area of 160.7 m2 g&minus, 1. The material delivers an initial capacity of 211 mAh g&minus, 1 with high Coulombic efficiency of 99% and 82% capacity retention after 100 cycles. Thus, &alpha, KyMnO2 synthesized via a green process exhibits very promising electrochemical performance in terms of initial capacity, cycling stability and rate capability.

Published
2020
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44. Electrochemical characterization of the artificial metalloenzyme papain-[(η6-arene)Ru(1,10-phenanthroline)Cl]+

Author

Jakub Šebera, Štěpánka Nováková Lachmanová, Barisa Talbi, Magdaléna Hromadová, Michèle Salmain, Lubomír Pospíšil, J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL), 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), Chemical Biology (CHEMBIO), and Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769)

Subjects
[CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemical Engineering, Phenanthroline, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Transfer hydrogenation, Electrochemistry, 01 natural sciences, Combinatorial chemistry, 3. Good health, 0104 chemical sciences, Analytical Chemistry, Dielectric spectroscopy, Catalysis, Papain, chemistry.chemical_compound, chemistry, [CHIM.COOR]Chemical Sciences/Coordination chemistry, 0210 nano-technology, Voltammetry, ComputingMilieux_MISCELLANEOUS, Conjugate
Abstract

Electrochemical properties were studied for [(η6-arene)Ru(1,10-phenanthroline)Cl]Cl (arene = C6H5(CH2)2NHCOCH2Cl) organometallic complex 1, protein Papain PAP and its conjugate with organometallic complex 1-PAP. The latter can serve as an artificial metalloenzyme with catalytic activity in transfer hydrogenation. This work demonstrates that AC voltammetry and electrochemical impedance spectroscopy can be used as fast tools to screen the catalytic ability of 1-PAP electrochemically by studies of the catalytic hydrogen evolution reaction (HER). Proteins are known to catalyze this process, but we have shown that additional HER signal associated with the catalytic activity of 1 is observed for its conjugate with Papain 1-PAP.

Published
2020
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45. Enhancement of the biocompatibility by surface nitriding of a low‐modulus titanium alloy for dental implant applications

Author

Sylvie Tricot-Doleux, T. Gloriant, Silviu Iulian Drob, Pascal Pellen-Mussi, Cora Vasilescu, Fabienne Pérez, D.M. Gordin, Yvan Bédouin, Dominique Chauvel-Lebret, CHU Pontchaillou [Rennes], 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), Centre hospitalier universitaire de Nantes (CHU Nantes), Institute of Physical Chemistry 'Ilie Murgulescu' Romanian Academy (ICF), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and 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)

Subjects
titanium alloy, [SDV.BIO]Life Sciences [q-bio]/Biotechnology, Materials science, Biocompatibility, Niobium, medicine.medical_treatment, Alloy, Biomedical Engineering, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, Corrosion, Biomaterials, Mice, biocompatibility, Cell Line, Tumor, Materials Testing, Alloys, medicine, Animals, Humans, [CHIM]Chemical Sciences, Composite material, Dental implant, Dental Implants, Titanium, surface nitriding, corrosion resistance, Low modulus, technology, industry, and agriculture, Titanium alloy, low modulus, 021001 nanoscience & nanotechnology, 0104 chemical sciences, superficial hardness, engineering, 0210 nano-technology, Layer (electronics), Nitriding
Abstract

To enhance their longevity, dental implants must be highly biocompatible and must have a low elastic modulus close to that of the bone. They must also possess a high superficial hardness and a high corrosion resistance. For these reasons, a recently developed low-modulus Ti-27Nb alloy with nontoxic elements was treated by gas nitriding at high temperature in this study. A very thin nitrided layer of 0.5 μm in thickness followed by an enriched nitrogen zone was observed. Consequently, a very high hardness evaluated at about 1800 HV was obtained in surface, which represents an increase of 4-5 times the hardness of the non-nitrided alloy. This superficial hardness was experimentally observed to decrease up to 800 nm in depth from the surface to the core. The low modulus of Ti-27Nb (evaluated at 55 GPa, which is twice lower than the commercially pure titanium) was not affected by the surface nitriding treatment. A better corrosion resistance was observed and a significant decrease in ion release rates for the nitrided alloy (ion release of 1.41 ng/cm2 compared to the 163.58 ng/cm2 obtained for the commercially pure titanium at pH = 7.48 in artificial Carter-Brugirard saliva). The cytocompatibility was not compromised and the cell viability performed on human osteoblasts, fibroblastic cells, and epithelial cells was enhanced on the nitrided surface in comparison with the non-nitrided surface. These combined properties make the nitrided Ti-27Nb alloy a good candidate for dental implant applications. © 2018 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater 107B: 1483-1490, 2019.

Published
2018
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46. Sn-BEA zeolites prepared by two-step postsynthesis method: Physicochemical properties and catalytic activity in processes based on MPV reduction

Author

Jan Żukrowski, Yannick Millot, Pavlo I. Kyriienko, Jacek Gurgul, Nataliia Popovych, Laetitia Valentin, Sergiy O. Soloviev, Robert P. Socha, Stanislaw Dzwigaj, L.V. Pisarzhevsky Institute of Physical Chemistry of the NAS of Ukraine, National Academy of Sciences of Ukraine (NASU), Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Jerzy Haber Institute of Catalysis and Surface Chemistry, Polska Akademia Nauk = Polish Academy of Sciences (PAN), Academic Centre for Materials and Nanotechnology, and AGH University of Science and Technology [Krakow, PL] (AGH UST)

Subjects
chemistry.chemical_classification, Isobutanol, Cyclohexanol, Cyclohexanone, Alcohol, Ether, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Aldehyde, 0104 chemical sciences, Catalysis, chemistry.chemical_compound, chemistry, Mechanics of Materials, Organic chemistry, General Materials Science, 0210 nano-technology, Zeolite, Tin BEA Zeolite Postsynthesis Lewis acidic sites Tandem process
Abstract

International audience; Sn0.5SiBEA and Sn2.0SiBEA zeolites obtained by two-step postsynthesis method were characterized by several physicochemical techniques (namely, NMR, Mössbauer, XPS, DR UV-vis and IR spectroscopies) and used in the study of Meerwein–Ponndorf–Verley (MPV) reduction as well as with the subsequent reaction of etherification, that is, conversion of (i) cyclohexanone with 2-propanol, (ii) 4-methoxybenzaldehyde with 2-butanol, and (iii) HMF with butyl alcohols (1-butanol, 2-butanol or isobutanol). The results have shown that in the case of cyclohexanone, MPV reduction to cyclohexanol occurs on both Sn0.5SiBEA and Sn2.0SiBEA zeolite catalysts with a higher degree of conversion in the presence of Sn2.0SiBEA. For 4-methoxybenzaldehyde a tandem process was observed consisting of MPV reduction with 2-butanol to 4-methoxybenzylalcohol followed by its etherification with 2-butanol to 4-methoxybenzyl sec-butyl ether. Higher conversion of aldehyde was achieved on the catalyst with higher amount of tin. The zeolites were active in HMF conversion with butyl alcohols. However, a tandem process including MPV reduction with the next formation of furanic diether was achieved only in the presence of secondary alcohol at test conditions.

Published
2018
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47. Supramolecular Assembly of Planar Systems from Modular Molecules with a Given Hydrophilic–Lipophilic Balance: Film Sensors with an Anthraquinone Signal Group

Author

Elizaveta V. Ermakova, L. V. Ermakova, A. Yu. Tsivadze, Vladimir V. Arslanov, Alla Bessmertnykh-Lemeune, Michel Meyer, A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences [Moscow] (RAS), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), Centre National de la Recherche Scientifique (CNRS)-Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC), and Russian Foundation for Basic Research 16-29-05272 17-53-16018 Program I.8 P of Presidium of the Russian Academy of Sciences

Subjects
mercury, Materials science, water, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, langmuir-blodgett-films, 01 natural sciences, Anthraquinone, orientation, Supramolecular assembly, chemistry.chemical_compound, Planar, Monolayer, Materials Chemistry, [CHIM]Chemical Sciences, Molecule, arrays, [PHYS]Physics [physics], Organic Chemistry, Metals and Alloys, 021001 nanoscience & nanotechnology, Copper, 0104 chemical sciences, Surfaces, Coatings and Films, Hydrophilic-lipophilic balance, monolayers, chemistry, Chemical engineering, copper, derivatives, heavy-metal ions, 0210 nano-technology, Selectivity
Abstract

International audience; This work presents an original approach to obtaining highly sensitive ultrathin film sensors that allows molecular design of surface-active modular molecules by completing a signal anthraquinone block with hydrophobic radicals and polar receptor groups, with their number and size provided in accordance with the sensor type. An important advantage of the suggested approach is that it not only allows the functioning of sensors in the aqueous medium, but also their manufacturing (supramolecular assembly). The key regularity of ligands of the suggested series is selectivity with respect to mercury and copper cations. Application of amphipilic ligands in film liquid (Langmuir monolayers) and solid-state (Langmuir-Blodgett films) sensors allowed developing optical sensors for mercury and copper cations with the detection limit, as dependent on the sensor type, varying from several to hundredths of ppm.

Published
2018
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48. Aqueous electrochemical energy storage system based on phenanthroline- and anthraquinone-modified carbon electrodes

Author

Galyna Shul, Nicolas Donzel, Daniel Bélanger, Mona Amiri, Institute of Physical Chemistry, Polish Academy of Sciences (PAN), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), 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), Département de Chimie [Montréal], and Université du Québec à Montréal = University of Québec in Montréal (UQAM)

Subjects
Materials science, General Chemical Engineering, Phenanthroline, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, Electrolyte, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, Anthraquinone, 0104 chemical sciences, chemistry.chemical_compound, Adsorption, chemistry, Electrode, medicine, [CHIM]Chemical Sciences, 0210 nano-technology, Carbon, ComputingMilieux_MISCELLANEOUS, Activated carbon, medicine.drug
Abstract

This manuscript reports the electrochemical behaviour of electrochemical energy storage system based on carbon-based electrodes modified with phenanthroline and anthraquinone molecules, respectively. The composite electrodes consist of activated carbon powder modified with phenanthroline or anthraquinone molecules by the diazonium chemistry. The phenanthroline-modified carbon used to prepare the composite electrode was characterized by elemental analysis, X-ray photoelectron spectroscopy, thermogravimetric analysis coupled to infrared spectrometry, and nitrogen gas adsorption. Phenanthroline-modified carbon composite electrode exhibited redox activity in aqueous acidic electrolyte around 0.4 V vs. Ag/AgCl. Consequently, it was used as positive electrode in electrochemical energy storage system with an anthraquinone-modified carbon negative electrode. Pre-polarization of both electrodes was needed to take full advantage of the charge storage properties of the grafted species and to reach the potential range of their redox activity upon charge/discharge cycling. This pre-treatment also enabled an increase of the operating voltage cell to 1.0 V in aqueous 1 M H2SO4 electrolyte.

Published
2021
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49. Interplay of entanglement and association effects on the dynamics of semidilute solutions of multisticker polymer chains

Author

Tsutomu Indei, Tetsuharu Narita, Maksim Shivokhin, Jay D. Schieber, Axel Habicht, Laurence Talini, Sebastian Seiffert, Illinois Institute of Technology (IIT), Sciences et Ingénierie de la Matière Molle (SIMM), Université Pierre et Marie Curie - Paris 6 (UPMC)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institute of Physical Chemistry, Johannes Gutenberg-Universitat Mainz, Johannes Gutenberg - Universität Mainz = Johannes Gutenberg University (JGU), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)

Subjects
chemistry.chemical_classification, Mechanical Engineering, Modulus, 02 engineering and technology, Quantum entanglement, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Viscoelasticity, 0104 chemical sciences, Condensed Matter::Soft Condensed Matter, Classical mechanics, Chain (algebraic topology), chemistry, Mechanics of Materials, Chemical physics, General Materials Science, Specular reflection, 0210 nano-technology, Constant (mathematics), [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], Elastic modulus, ComputingMilieux_MISCELLANEOUS
Abstract

We analyze the effects of polymer concentration, Cp, and physical crosslinking ratio, rc, on the linear viscoelasticity of lightly entangled, linear, associating polymers with multiple crosslinkable groups along the chain backbone. To accomplish this goal, we utilize three novel tools: a robust tunable chemistry based on electrophilic methacryl-succinimidyl modified poly(N-isopropylacrylamide); a modified state-of-the-art entanglement theory, called the discrete slip-link molecular model; and a novel experimental technique, surface fluctuation specular reflection. This experimental technique allows the extraction of the complex viscoelastic modulus covering up to six decades of frequency, from the sample's surface fluctuations at constant temperature. We demonstrate that our theoretical model with a consistent set of parameters can qualitatively reproduce the observed features of the complex viscoelastic modulus over the entire probed frequency range. Furthermore, the effects of Cp and rc on the viscoelas...

Published
2017
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50. Hierarchical templating in deposition of semi-covalently imprinted inverse opal polythiophene film for femtomolar determination of human serum albumin

Author

Paweł Borowicz, Marcin Dabrowski, Francis D'Souza, Piyush Sindhu Sharma, Alexander Kuhn, Wojciech Lisowski, Krzysztof Noworyta, Wlodzimierz Kutner, Maciej Cieplak, Institute of Physical Chemistry Polish Academy of Sciences, Institut des Sciences Moléculaires (ISM), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Université Sciences et Technologies - Bordeaux 1-Université Montesquieu - Bordeaux 4-Institut de Chimie du CNRS (INC), and Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Polymers, Biomedical Engineering, Biophysics, Serum Albumin, Human, Nanotechnology, Biosensing Techniques, Thiophenes, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Molecular Imprinting, chemistry.chemical_compound, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Electrochemistry, medicine, Humans, [CHIM]Chemical Sciences, Molecule, Derivatization, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Molecularly imprinted polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, General Medicine, Polymer, Colloidal crystal, 021001 nanoscience & nanotechnology, Human serum albumin, 0104 chemical sciences, body regions, chemistry, Chemical engineering, Covalent bond, Polythiophene, 0210 nano-technology, Biotechnology, medicine.drug
Abstract

Nanostructured artificial receptor materials with unprecedented hierarchical structure for determination of human serum albumin (HSA) are designed and fabricated. For that purpose a new hierarchical template is prepared. This template allowed for simultaneous structural control of the deposited molecularly imprinted polymer (MIP) film on three length scales. A colloidal crystal templating with optimized electrochemical polymerization of 2,3′-bithiophene enables deposition of an MIP film in the form of an inverse opal. Thickness of the deposited polymer film is precisely controlled with the number of current oscillations during potentiostatic deposition of the imprinted poly(2,3′-bithiophene) film. Prior immobilization of HSA on the colloidal crystal allows formation of molecularly imprinted cavities exclusively on the internal surface of the pores. Furthermore, all binding sites are located on the surface of the imprinted cavities at locations corresponding to positions of functional groups present on the surface of HSA molecules due to prior derivatization of HSA molecules with appropriate functional monomers. This synergistic strategy results in a material with superior recognition performance. Integration of the MIP film as a recognition unit with a sensitive extended-gate field-effect transistor (EG-FET) transducer leads to highly selective HSA determination in the femtomolar concentration range.

Published
2017
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