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149 results on '"Matériaux Hybrides et Nanomatériaux (LCMCP-MHN)"'

1. Revealing the Elusive Structure and Reactivity of Iron Boride α-FeB

Author: Fernando Igoa Saldaña, Emile Defoy, Daniel Janisch, Gwenaëlle Rousse, Pierre-Olivier Autran, Anissa Ghoridi, Amandine Séné, Marzena Baron, Leopoldo Suescun, Yann Le Godec, David Portehault, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Design et étude de nouveaux matériaux à propriété remarquables [IMPMC] (IMPMC_DEMARE), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Collège de France - Chaire Chimie du solide et énergie, Chimie du solide et de l'énergie (CSE), Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), European Synchroton Radiation Facility [Grenoble] (ESRF), Laboratorio de Cristalografıa, Estado Solido y Materiales [UCUR] (Cryssmat-Lab), Universidad de la República [Montevideo] (UDELAR), and Doctoral School ED397ESRF proposal MA-5188
Subjects: Inorganic Chemistry, crystal structure, borides, intergrowth, in situ XRD, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Physical and Theoretical Chemistry, FAULTS
Abstract: International audience; Crystal structures can strongly deviate from bulk states when confined into nanodomains. These deviations may deeply affect properties and reactivity and then call for a close examination. In this work, we address the case where extended crystal defects spread through a whole solid and then yield an aperiodic structure and specific reactivity. We focus on iron boride, α-FeB, whose structure has not been elucidated yet, thus hindering the understanding of its properties. We synthesize the two known phases, α-FeB and β-FeB, in molten salts at 600 and 1100 °C, respectively. The experimental X-ray diffraction (XRD) data cannot be satisfactorily accounted for by a periodic crystal structure. We then model the compound as a stochastic assembly of layers of two structure types. Refinement of the powder XRD pattern by considering the explicit scattering interference of the different layers allows quantitative evaluation of the size of these domains and of the stacking faults between them. We, therefore, demonstrate that α-FeB is an intergrowth of nanometer-thick slabs of two structure types, β-FeB and CrB-type structures, in similar proportions. We finally discuss the implications of this novel structure on the reactivity of the material and its ability to perform insertion reactions by comparing the reactivities of α-FeB and β-FeB as reagents in the synthesis of a model layered material: Fe2AlB2. Using synchrotron-based in situ X-ray diffraction, we elucidate the mechanisms of the formation of Fe2AlB2. We highlight the higher reactivity of the intergrowth α-FeB in agreement with structural relationships.
Published: 2023

2. In Operando Spectroscopic Ellipsometry Investigation of MOF Thin Films for the Selective Capture of Acetic Acid

Author: Sanchari Dasgupta, Subharanjan Biswas, Kevin Dedecker, Eddy Dumas, Nicolas Menguy, Bruno Berini, Bertrand Lavedrine, Christian Serre, Cédric Boissière, Nathalie Steunou, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Centre de Recherche sur la Conservation (CRC ), Muséum national d'Histoire naturelle (MNHN)-Ministère de la Culture et de la Communication (MCC)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and This work was supported by the Ecole Universitaire de recherche PSGS HCH Humanities, Creation, Heritage, Investissement d’Avenir ANR-17-EURE-0021 - Fondation des sciences du patrimoine. This work has been sponsored by the Ile-de-France Region in the framework of Respore, the Île-de-France network of Excellence in Porous Solids. The authors acknowledge Ali Saad for SEM experiments.
Subjects: Ellipsometry, adsorption, Thin films, [SDE]Environmental Sciences, [CHIM]Chemical Sciences, General Materials Science, Volatile organic compounds, MOFs
Abstract: International audience; The emission of polar volatile organic compounds (VOCs) is a major worldwide concern of air quality and equally impacts the preservation of cultural heritage (CH). The challenge is to design highly efficient adsorbents able to selectively capture traces of VOCs such as acetic acid (AA) in the presence of relative humidity (RH) normally found at storage in museums (40-80%). Although the selective capture of VOCs over water is still challenging, Metal-Organic Frameworks (MOFs) possess highly tunable features (Lewis, Bronsted or redox metal sites, functional groups, hydrophobicity…) suitable to selectively capture a large variety of VOCs. In this context, we have explored the adsorption efficiency of a series of MOFs thin films (ZIF-8(Zn), MIL-101(Cr) and UiO-66(Zr)-2CF3) for the selective capture of AA based on a UV/Vis and FT-IR spectroscopic ellip-sometry in operando study (2-6% of relative pressure of AA under 40% of RH), namely conditions close to the realistic envi-ronmental storage conditions of cultural artefacts. For that purpose, optical quality thin films of MOFs were prepared by dip-coating and their AA adsorption capacity and selectivity were evaluated under humid conditions by measuring the variation of the refractive index as a function of the vapor pressures while the chemical nature of the co-adsorbed analytes (water and AA) was identified by FT-IR ellipsometry. While thin films of ZIF-8(Zn) strongly degraded when exposed to AA/water va-pors, films of MIL-101(Cr) and UiO-66(Zr)-2CF3 present a high chemical stability under those conditions. It was shown that MIL-101(Cr) presents a high AA adsorption capacity due to its high pore volume, but exhibits a poor AA adsorption selectivi-ty under humid conditions. In contrast, UiO-66(Zr)-2CF3 was shown to overpass MIL-101(Cr) in terms of AA/ H2O adsorp-tion selectivity and AA adsorption/desorption cycling stability thanks to its high hydrophobic character, suitable pore size for adequate confinement and specific interactions.
Published: 2023

3. Molten Salts‐Driven Discovery of a Polar Mixed‐Anion 3D framework at the nanoscale: Zn4Si2O7Cl2, Charge Transport and Photoelectrocatalytic Water Splitting

Author: Kumar, Ram, Song, Yang, Ghoridi, Anissa, Boullay, Philippe, Rousse, Gwenaelle, Gervais, Christel, Diogo, Cristina Coelho, Kabbour, Houria, Sassoye, Capucine, Beaunier, Patricia, Castaing, Victor, Viana, Bruno, Ruiz Gonzalez, Maria Luisa, Calbet, José Gonzalez, Laberty-Robert, Christel, Portehault, David, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Chimie du solide et de l'énergie (CSE), Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Fédération de Chimie et Matériaux de Paris-Centre (FCMat), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Recherche de Chimie Paris (IRCP), 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)-Ministère de la Culture (MC), Université Paris sciences et lettres (PSL), Universidad Complutense de Madrid = Complutense University of Madrid [Madrid] (UCM), Reactive Materials for Electrochemical Systems (LCMCP-RMES ), and CNRS-CEA METSA network, Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357, GENCI-IDRIS (Grant 097535). Région Ile de France - SESAME
Subjects: electron crystallography, mixed anions, photoelectrocatalysis, molten salts, [CHIM.CRIS]Chemical Sciences/Cristallography, oxychloride, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: International audience; Mixed-anion compounds widen the chemical space of attainable materials compared to single anionic compounds, but the exploration of their structural diversity is limited by common synthetic paths. Especially, oxychlorides rely mainly on layered structures, which suffer from low stability during photo(electro)catalytic processes. Herein we report a strategy to design a new polar 3D tetrahedral framework with composition Zn4Si2O7Cl2. We use a molten salt medium to enable low temperature crystallization of nanowires of this new compound, by relying on tetrahedral building units present in the melt to build the connectivity of the oxychloride. These units are combined with silicon-based connectors from a non-oxidic Zintl phase to enable precise tuning of the oxygen content. This structure brings high chemical and thermal stability, as well as strongly anisotropic hole mobility along the polar axis. These features, associated with the ability to adjust the transport properties by doping, enable to tune water splitting properties for photoelectrocatalytic H2 evolution and water oxidation. This work then paves the way to a new family of mixed-anion solids
Published: 2023

4. Liquid Processing of Bismuth–Silica Nanoparticle/Aluminum Matrix Nanocomposites for Heat Storage Applications

Author: Binghua Ma, Walid Baaziz, Léo Mazerolles, Ovidiu Ersen, Bernard Sahut, Clément Sanchez, Stéphane Delalande, David Portehault, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Stellantis - PSA Centre Technique de Vélizy, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), 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), Portehault, David, and Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE)
Subjects: heat storage, [CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, phase change, aluminum, bismuth, nanoparticles, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, composites, core−shell
Abstract: International audience; Metal matrix nanocomposites encompassing low-melting point metal nano-inclusions are promising candidates for thermal regulation of devices at high temperature. They are usually processed by solid-state routes that provide access to a limited range of materials and are hardly compatible with complex shaping processes and with large-scale applications. Herein, we develop a liquid-phase processing technique to design aluminum matrix nanocomposites made of phase change nanoparticles, using bismuth nanoparticles as a proof-of-concept. The bismuth nanoparticles derived from colloidal chemistry are first encapsulated in a silica shell and then dispersed by ultrasonication into molten aluminum. Using X-ray diffraction, electron microscopy, and X-ray photoelectron spectroscopy, we probe the evolution of the bismuth particles and of the inorganic shell. We demonstrate that the silica shell acts as a barrier against extensive coalescence of particles during the dispersion process, thus enabling a decrease and a widening of the phase change temperature range.
Published: 2022

5. Advanced Functional Hybrid Proton Exchange Membranes Robust and Conductive at 120 °C

Author: Jason Richard, Fatima Haidar, Madeline K. Alzamora, Manuel Maréchal, Natalia Rovira, Christophe Vacquier, Clément Sanchez, Christel Laberty‐Robert, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), 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), Symbio, Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut d’Etudes Avancées de l’Université de Strasbourg - Institute for Advanced Study (USIAS), Université de Strasbourg (UNISTRA), Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), and Université de Montpellier (UM)
Subjects: Mechanics of Materials, Mechanical Engineering, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience
Published: 2022

6. Periodic nanoporous inorganic patterns directly made by self-ordering of cracks

Author: Mateusz Odziomek, Fanny Thorimbert, Cedric Boissiere, Glenna L. Drisko, Stephane Parola, Clement Sanchez, Marco Faustini, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB), Université de Bordeaux (UB)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-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), and The European Research Council (ERC) under European Union’s Horizon 2020 Programme (Grant Agreement no. 803220, TEMPORE). The College de France for financial support and the Foundation for Polish Science (FNP) for a START scholarship.
Subjects: patterning, Mechanics of Materials, Mechanical Engineering, porous films, inorganic, crack, photonics, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Solution-processed inorganic nanoporous films are key components for the vast spectrum of applications ranging from dew harvesting to solar cells. Shaping them into complex architectures required for advanced functionality, often need time-consuming or expensive fabrication. In this work, we show how crack formation is harnessed to pattern porous inorganic films in a single step and without using lithography. We developed aqueous ink formulations that, in the presence of polymeric latexes, enable evaporation-induced, defect-free periodic arrays of cracks with tunable dimensions over several centimeters. The ink formulation strategy was generalized to more than ten inorganic materials including simple and binary porous oxide and metallic films covering a whole spectrum of properties including insulator, photocatalytic, electrocatalytic, conductive or electrochromic materials. Notably, this approach enables three-dimensional self-assembly of cracks by stacking several layers of different compositions, yielding periodic assemblies of polygonal shapes and Janus-type patterns. The crack patterned periodic arrays of nanoporous TiO2 diffract light, and are used as temperature-responsive diffraction grating sensors. More broadly, this method represents a unique example of self-assembly process leading to long-range order (over several cm) in a robust and controlled way.
Published: 2022

7. In situ liquid transmission electron microscopy reveals self-assembly-driven nucleation in radiolytic synthesis of iron oxide nanoparticles in organic media

Author: Nathaly Ortiz Peña, Dris Ihiawakrim, Sorina Creţu, Geoffrey Cotin, Céline Kiefer, Sylvie Begin-Colin, Clément Sanchez, David Portehault, Ovidiu Ersen, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Portehault, David
Subjects: [CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, Aucun, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry
Abstract: International audience; We have investigated the early stages of formation of iron oxide nanoparticles from iron stearate precursors in the presence of sodium stearate in an organic solvent by in situ liquid phase transmission electron microscopy (IL-TEM). Before nucleation, we have evidenced the spontaneous formation of vesicular assemblies made of iron polycation-based precursors sandwiched between stearate layers. Nucleation of iron oxide nanoparticles occurs within the walls of the vesicles, which subsequently collapse upon consumption of the iron precursors and growth of the nanoparticles. We then evidenced that fine control of the electron dose, and therefore of the local concentration of reactive iron species in the vicinity of the nuclei, enables controlling crystal growth and selecting the morphology of the resulting iron oxide nanoparticles. Such direct observation of the nucleation process templated by vesicular assemblies in a hydrophobic organic solvent sheds new light on the formation process of metal oxide nanoparticles and therefore opens ways for the synthesis of inorganic colloidal systems with tunable shape and size.
Published: 2022

8. Geoinspired syntheses of materials and nanomaterials

Author: David Portehault, Isabel Gómez-Recio, Marzena A. Baron, Valentina Musumeci, Cyril Aymonier, Virgile Rouchon, Yann Le Godec, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB), Université de Bordeaux (UB)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), IFP Energies nouvelles (IFPEN), Cosmochimie [IMPMC] (IMPMC_COSMO), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and This work has been supported by the European Research Council (ERC) Consolidator Grant GENESIS under the European Union's Horizon 2020 research and innovation program (grant agreement no 864850).
Subjects: Water, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Nanostructures
Abstract: International audience; The search for new materials is intimately linked to the development of synthesis methods. In the current urge for the sustainable synthesis of materials, taking inspiration from Nature's ways to process matter appears as a virtuous approach. In this review, we address the concept of geoinspiration for the design of new materials and the exploration of new synthesis pathways. In geoinspiration, materials scientists take inspiration from the key features of various geological systems and processes occurring in nature, to trigger the formation of artificial materials and nanomaterials. We discuss several case studies of materials and nanomaterials to highlight the basic geoinspiration concepts underlying some synthesis methods: syntheses in water and supercritical water, thermal shock syntheses, molten salt synthesis and high pressure synthesis. We show that the materials emerging from geoinspiration exhibit properties differing from materials obtained by other pathways, thus demonstrating that the field opens up avenues to new families of materials and nanomaterials. This review focuses on synthesis methodologies, by drawing connections between geosciences and materials chemistry, nanosciences, green chemistry, and environmental sciences.
Published: 2022

9. Hydroxyapatites as Versatile Inorganic Hosts of Unusual Pentavalent Manganese Cations

Author: María Hernando, José M. González-Calbet, Marina Parras, Christel Laberty-Robert, Aurea Varela, Gwenaëlle Rousse, José Luis Martínez, Laura Serrador, David Portehault, María Teresa Fernández-Díaz, Francisco Gonell, E. Matesanz, Clément Sanchez, Isabel Gómez-Recio, Almudena Torres-Pardo, Universidad Complutense de Madrid = Complutense University of Madrid [Madrid] (UCM), Institut Laue-Langevin (ILL), ILL, Laboratoire des Sciences du Numérique de Nantes (LS2N), IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-École Centrale de Nantes (ECN)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sorbonne Université (SU), Chaire Chimie des matériaux hybrides, and Reactive Materials for Electrochemical Systems (LCMCP-RMES )
Subjects: Chemistry, General Chemical Engineering, chemistry.chemical_element, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, General Chemistry, Manganese, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Polymer chemistry, Materials Chemistry, Hydroxyapatites, 0210 nano-technology
Abstract: International audience; Contrary to molecular species, only very few solids are reported to host manganese (V) species. Herein, we report three new compounds with a hydroxyapatite structural backbone built on the Mn V O 4 3− anion: Sr 5 [(Mn 1−x Si x)O 4 ] 3 (OH) 1−3x (x =0 and 0.053), Sr 5 (MnO 4) 3 (OH) 1−y F y (y = 0.90), and Sr 5 [(Mn 1−x Si x)-O 4 ] 3 F 1−3x (x = 0.058). These solids are fully characterized using powder X-ray and neutron powder diffraction, scanning transmission electron microscopy, electron energy loss spectroscopy (EELS), thermogravimetric analysis, and magnetic measurements. Especially, we report for the first time EELS Mn−L 2,3 spectra of manganese with the oxidation state (V). Contrary to other Mn(V) oxides, these solids and the nominal compound Sr 5 (MnO 4) 3 OH do not comprise Ba 2+ cations but rely only on Sr 2+ cations, showing that barium is not a required element to stabilize Mn(V) species in inorganic solids. We show that by tuning soft chemistry conditions on the one hand and post-treatment topological transformation conditions on the other hand, Mn(V) and hydroxyl groups can be substituted by Si(IV) and fluoride ions, respectively. Hence, we deliver solids with a potentially wide composition range. These compounds show significant oxygen anionic conduction, thus suggesting the emergence of new functional materials built from high-oxidation state manganese cations.
Published: 2020

10. Inorganic phosphate in growing calcium carbonate abalone shell suggests a shared mineral ancestral precursor

Author: Widad Ajili, Camila B. Tovani, Justine Fouassier, Marta de Frutos, Guillaume Pierre Laurent, Philippe Bertani, Chakib Djediat, Frédéric Marin, Stéphanie Auzoux-Bordenave, Thierry Azaïs, Nadine Nassif, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Molécules de Communication et Adaptation des Micro-organismes (MCAM), Muséum national d'Histoire naturelle (MNHN)-Centre National de la Recherche Scientifique (CNRS), Biogéosciences [UMR 6282] (BGS), Université de Bourgogne (UB)-Centre National de la Recherche Scientifique (CNRS), Biologie des Organismes et Ecosystèmes Aquatiques (BOREA), Université de Caen Normandie (UNICAEN), and Normandie Université (NU)-Normandie Université (NU)-Muséum national d'Histoire naturelle (MNHN)-Institut de Recherche pour le Développement (IRD)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université des Antilles (UA)
Subjects: Calcium Phosphates, [PHYS]Physics [physics], Minerals, Multidisciplinary, [SDV]Life Sciences [q-bio], Gastropoda, Carbonates, General Physics and Astronomy, General Chemistry, General Biochemistry, Genetics and Molecular Biology, Calcium Carbonate, Phosphates, Animals, [CHIM]Chemical Sciences
Abstract: The presence of phosphate from different origins (inorganic, bioorganic) is found more and more in calcium carbonate-based biominerals. Phosphate is often described as being responsible for the stabilization of the transient amorphous calcium carbonate phase. In order to specify the composition of the mineral phase deposited at the onset of carbonated shell formation, the present study investigates, down to the nanoscale, the growing shell from the European abalone Haliotis tuberculata, using a combination of solid state nuclear magnetic resonance, scanning transmission electron microscope and spatially-resolved electron energy loss spectroscopy techniques. We show the co-occurrence of inorganic phosphate with calcium and carbonate throughout the early stages of abalone shell formation. One possible hypothesis is that this first-formed mixed mineral phase represents the vestige of a shared ancestral mineral precursor that appeared early during Evolution. In addition, our findings strengthen the idea that the final crystalline phase (calcium carbonate or phosphate) depends strongly on the nature of the mineral-associated proteins in vivo.
Published: 2022

11. Native Collagen: Electrospinning of Pure, Cross-Linker-Free, Self-Supported Membrane

Author: Nicolas Debons, Frank Wien, Christel Laberty-Robert, Julien Rodrigues da Silva, Carole Aimé, Marie-Claire Schanne-Klein, Natacha Krins, Yong Chen, Christophe Hélary, Laurent Muller, Marion Marchand, Dounia Dems, Matériaux et Biologie (LCMCP-MATBIO), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Centre interdisciplinaire de recherche en biologie (CIRB), Labex MemoLife, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Collège de France (CdF (institution))-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'optique et biosciences (LOB), École polytechnique (X)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Collège de France (CdF (institution))-École normale supérieure - Paris (ENS Paris), and Université Paris sciences et lettres (PSL)-Collège de France (CdF (institution))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)
Subjects: hierarchical organization, Biomedical Engineering, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biomaterials, Tissue engineering, Native state, second harmonic generation microscopy, Cross linker, electrospinning, chemistry.chemical_classification, Biomolecule, Biochemistry (medical), [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Second Harmonic Generation Microscopy, 021001 nanoscience & nanotechnology, Electrospinning, 0104 chemical sciences, Membrane, chemistry, extra-cellular matrix, tissue engineering, Collagen, 0210 nano-technology
Abstract: International audience; Rebuilding biological environments is crucial when facing the challenges of fundamental and biomedical research. Thus, preserving the native state of biomolecules is essential. We use electrospinning (ES), which is an extremely promising method for the preparation of fibrillar membranes to mimic the ECM of native tissues. Here, we report for the first time (1) the ES of pure and native collagen into a self-supported membrane in absence of crosslinker and polymer support, (2) the preservation of the membrane integrity in hydrated media in absence of crosslinker and (3) the preservation of the native molecular structure and recovery of the hierarchical assembly of collagen. We use a multiscale approach to characterize collagen native structure at the molecular level using circular dichroism, and to investigate collagen hierarchical organization within the self-supported membrane using a combination of multiphoton and electron microscopies. Finally, we show that the membranes are perfectly suited for cell adhesion and spreading, making them very promising candidates for the development of biomaterials and finding applications in biomedical research.
Published: 2022

12. Nanoscale Analysis of Randall’s Plaques by Electron Energy Loss Spectromicroscopy: Insight in Early Biomineral Formation in Human Kidney

Author: Michael Walls, Dominique Bazin, Marie-Christine Verpont, Marta de Frutos, Odile Stéphan, Nadine Nassif, Emmanuel Letavernier, Michel Daudon, Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Des Maladies Rénales Rares aux Maladies Fréquentes, Remodelage et Réparation, Institut National de la Santé et de la Recherche Médicale (INSERM)-Sorbonne Université (SU), CHU Tenon [AP-HP], Sorbonne Université (SU)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Calcium Phosphates, kidney, Surface Properties, [SDV]Life Sciences [q-bio], calcium carbonate nanoparticles, General Physics and Astronomy, chemistry.chemical_element, Electrons, Spectroscopy, Electron Energy-Loss, 02 engineering and technology, Calcium, 010402 general chemistry, [SDV.MHEP.UN]Life Sciences [q-bio]/Human health and pathology/Urology and Nephrology, 01 natural sciences, Kidney Calculi, chemistry.chemical_compound, calcium phosphate nanoparticles, medicine, Humans, Nanotechnology, General Materials Science, Particle Size, electron energy-loss spectroscopy, [PHYS]Physics [physics], Kidney Medulla, Biomineral formation, Electron energy, Vesicle, General Engineering, Human kidney, biomineralization, 021001 nanoscience & nanotechnology, medicine.disease, 0104 chemical sciences, chemistry, Biophysics, Carbonate, Randall’s plaques, 0210 nano-technology, Biomineralization, Calcification
Abstract: International audience; Idiopathic kidney stones originate mainly from calcium phosphate deposits at the tip of renal papillae, known as Randall’s plaques (RPs), also detected in most human kidneys without stones. However, little is known about the mechanisms involved in RP formation. The localization and characterization of such nano-sized objects in the kidney remains a real challenge making their study arduous. This study provides a nanoscale analysis of the chemical composition and morphology of incipient RPs, characterizing in particular the interface between the mineral and the surrounding organic compounds. Relying on data gathered from a calculi collection, the morphology and chemical composition of incipient calcifications in renal tissue was determined using spatially resolved electron energy-loss spectroscopy (EELS). We detected micro-calcifications and individual nano-calcifications found at some distance from the larger ones. Strikingly, concerning the smaller ones, we show that two types of nano-calcifications coexist: calcified organic vesicles and nanometric mineral granules mainly composed of calcium phosphate with carbonate in their core. Interestingly, some of these nano-calcifications present similarities with those reported in physiological bone or pathological cardiovascular biominerals, suggesting possible common formation mechanisms. However the high diversity of these nano-calcifications suggests that several mechanisms may be involved (nucleation on a carbonate core or on organic compounds). In addition, incipient RPs also appear to present specific features at larger scales revealing secondary calcified structures embedded in a fibrillar organic material. Our study proves that analogies exist between physiological and pathological biominerals and provides information to understand the physico-chemical processes involved in pathological calcification formation.
Published: 2020

13. Self-supporting carbon-rich SiOC ceramic electrodes for lithium-ion batteries and aqueous supercapacitors

Author: Gurpreet Singh, François Ribot, Christel Gervais, Shakir Bin Mujib, Department of Mechanical and Nuclear Engineering, Kansas State University, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), and Department of Mechanical and Nuclear Engineering [Manhattan]
Subjects: Supercapacitor, Materials science, General Chemical Engineering, [SPI.NRJ]Engineering Sciences [physics]/Electric power, chemistry.chemical_element, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, Electrochemical energy conversion, 0104 chemical sciences, X-ray photoelectron spectroscopy, chemistry, Chemical engineering, visual_art, Electrode, visual_art.visual_art_medium, Lithium, Ceramic, 0210 nano-technology, Carbon, Faraday efficiency
Abstract: International audience; Fabrication of precursor-derived ceramic fibers as electrodes for energy storage applications remains largely unexplored. Within this work, three little known polymer-derived ceramic (PDC)-based fibers are being studied systemically as potential high-capacity electrode materials for electrochemical energy devices. We report fabrication of precursor-derived SiOC fibermats via one-step spinning from various compositions of siloxane oligomers followed by stabilization and pyrolysis at 800 C. Electron microscopy, Raman, FTIR, XPS, and NMR spectroscopies reveal transformation from polymer to ceramic stages of the various SiOC ceramic fibers. The ceramic samples are a few microns in diameter with a free carbon phase embedded in the amorphous Si–O–C structure. The free carbon phase improves the electronic conductivity and provides major sites for ion storage, whereas the Si–O–C structure contributes to high efficiency. The self-standing electrodes in lithium-ion battery half-cells deliver a charge capacity of 866 mA.h.gelectrode-1 with a high initial coulombic efficiency of 72%. As supercapacitor electrode, SiOC fibers maintain 100% capacitance over 5000 cycles at a current density of 3 A.g-1.
Published: 2021

14. Spark plasma sintering of nanostructured ZnS ceramics: Grain growth control and improved hardness

Author: Julie Cédelle, Damien Bregiroux, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Energétique Mécanique Electromagnétisme (LEME), and Université Paris Nanterre (UPN)
Subjects: 010302 applied physics, Materials science, Mechanical Engineering, Metallurgy, Spark plasma sintering, Sintering, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Indentation hardness, Grain size, Grain growth, Mechanics of Materials, visual_art, 0103 physical sciences, visual_art.visual_art_medium, General Materials Science, Ceramic, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract: The densification and grain growth behavior of a ZnS nanopowder during spark plasma sintering (SPS) were investigated under the pressure of 125 MPa and constant heating rate of 25 °C min−1. At a sintering temperature of 550 °C, almost fully dense ZnS ceramics (98.2%) could be obtained with grain size as low as 75 nm. At higher temperature, ZnS is subject of a very important grain growth that is detrimental to the mechanical properties. A maximum Vickers microhardness of 4.2 GPa was measured, which is 70% higher than the current state of the art. Retaining the grain size below 100 nm appears to be the key to developing competitive ZnS functional ceramics.
Published: 2021

15. Ultrasound-Assisted Liquid-Phase Synthesis and Mechanical Properties of Aluminum Matrix Nanocomposites Incorporating Boride Nanocrystals

Author: Ma, Binghua, Gómez-Recio, Isabel, Gómez‐recio, Isabel, Mazerolles, L., Mazeran, Pierre‐emmanuel, Sanchez, Clément, Delalande, Stéphane, Portehault, David, 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), Stellantis France, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Roberval (Roberval), and Université de Technologie de Compiègne (UTC)
Subjects: Materials science, Nucleation, Nanoparticle, 02 engineering and technology, mechanical properties, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 01 natural sciences, Biomaterials, chemistry.chemical_compound, Boride, 0103 physical sciences, metal matrix nanocomposites, General Materials Science, ComputingMilieux_MISCELLANEOUS, Grain boundary strengthening, 010302 applied physics, Nanocomposite, boride nanoparticles, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Nanoindentation, 021001 nanoscience & nanotechnology, Grain size, Nanocrystal, Chemical engineering, chemistry, 0210 nano-technology, Biotechnology
Abstract: International audience; Incorporating boride nanocrystals could significantly impact the mechanical properties of aluminum alloys. Molten salts synthesis offers opportunities to fabricate superhard boride nanoparticles, which can sustain the harsh conditions during the liquid-phase design of metallic nanocomposites. Here hafnium diboride-aluminum nanocomposites are unveiled from molten salt-derived HfB2 nanoparticles sequentially dispersed in aluminum by ultrasound treatment. The structure and size of the nanocrystals are retained in the final nanocomposites, supporting their high chemical stability. Semicoherent interfaces between the nanoparticles and the matrix are then evidenced by TEM, suggesting that the nanocrystals could promote heterogeneous nucleation of Al and then limit the Al grain size to ≈20 µm. Nanoindentation measurements reveal significant grain boundary strengthening and grain refinement effects. It is finally shown that HfB2 nanoparticles also enable a decrease in matrix grain size and an increase in the hardness of the AlSi7Cu0.5Mg0.3 alloy. These proof-of-concept materials are paving the way to light-weight Al matrix nanocomposites doped by molten-salt synthesized nanoparticles.
Published: 2021

16. Dysprosium doping of Ca2MnO4: Effect on crystal structure at room temperature and thermal behavior

Author: M. Allani, D. Bregiroux, A. Bahezre, G. Wallez, Christel Laberty-Robert, Gwenaëlle Rousse, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Chimie du solide et de l'énergie (CSE), Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Recherche de Chimie Paris (IRCP), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ministère de la Culture (MC)
Subjects: Range (particle radiation), Materials science, Doping, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, Crystal structure, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, chemistry, Thermal, Thermoelectric effect, Dysprosium, [CHIM.CRIS]Chemical Sciences/Cristallography, General Materials Science, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract: Dysprosium-doped Ruddlesden−Popper calcium manganates with compositions of Ca2-xDyxMnO4 are potential candidates for high temperature thermoelectric applications. The effect of dysprosium doping on the crystal structure of Ca2-xDyxMnO4 at room temperature and its thermal behavior between RT and 800 °C were investigated in the range 0
Published: 2021

17. The origin of the high electrochemical activity of pseudo-amorphous iridium oxides

Author: Cédric Boissière, Marine Elmaalouf, Clément Sanchez, Mounib Bahri, Jean-Yves Piquemal, Mateusz Odziomek, Andrea Zitolo, Ovidiu Ersen, Benedikt Lassalle-Kaiser, Maxime Gayrard, Marion Giraud, Silvia Duran, Jennifer Peron, Marco Faustini, Cédric Tard, HAL-SU, Gestionnaire, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie moléculaire (LCM), École polytechnique (X)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Université de Strasbourg (UNISTRA)-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), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique
Subjects: [CHIM.INOR] Chemical Sciences/Inorganic chemistry, Materials science, Science, General Physics and Astronomy, chemistry.chemical_element, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Electrocatalyst, 01 natural sciences, Article, General Biochemistry, Genetics and Molecular Biology, law.invention, X-ray photoelectron spectroscopy, law, Oxidation state, Porous materials, Calcination, Iridium, Crystallization, [CHIM.MATE] Chemical Sciences/Material chemistry, Energy, Multidisciplinary, Structural properties, 010405 organic chemistry, Oxygen evolution, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 0104 chemical sciences, Amorphous solid, Chemical engineering, chemistry, 13. Climate action, Nanoparticles, Electrocatalysis
Abstract: Combining high activity and stability, iridium oxide remains the gold standard material for the oxygen evolution reaction in acidic medium for green hydrogen production. The reasons for the higher electroactivity of amorphous iridium oxides compared to their crystalline counterpart is still the matter of an intense debate in the literature and, a comprehensive understanding is needed to optimize its use and allow for the development of water electrolysis. By producing iridium-based mixed oxides using aerosol, we are able to decouple the electronic processes from the structural transformation, i.e. Ir oxidation from IrO2 crystallization, occurring upon calcination. Full characterization using in situ and ex situ X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and transmission electron microscopy allows to unambiguously attribute their high electrochemical activity to structural features and rules out the iridium oxidation state as a critical parameter. This study indicates that short-range ordering, corresponding to sub-2nm crystal size for our samples, drives the activity independently of the initial oxidation state and composition of the calcined iridium oxides., The origins of the superior catalytic activity of poorly crystallized Ir-based oxide material for the OER in acid is still under debate. Here, authors synthesize porous IrMo oxides to deconvolute the effect of Ir oxidation state from short-range ordering and show the latter to be a key factor.
Published: 2021

18. Interlayer Silylation of Layered Octosilicate with Organoalkoxysilanes: Effects of Tetrabutylammonium Fluoride as a Catalyst and the Functional Groups of Silanes

Author: Yuki Murakami, David Portehault, Atsushi Shimojima, Masakazu Koike, Michel Wong Chi Man, Masashi Yatomi, Nadège Rey, Clément Sanchez, Shohei Saito, Sophie Carenco, Carole Carcel, Hiroaki Wada, Kazuyuki Kuroda, Tokyo Institute of Technology [Tokyo] (TITECH), 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), University of Aizu [Japan] (UoA), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Collège de France (CdF (institution))
Subjects: Silanes, Silylation, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Tetrabutylammonium fluoride, 01 natural sciences, 0104 chemical sciences, Catalysis, Inorganic Chemistry, chemistry.chemical_compound, chemistry, Polymer chemistry, Octosilicate, [CHIM]Chemical Sciences, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021

19. Alkoxysilane effect in hybrid material: A comparison of pHEMA-TiO2 and pMAPTMS-TiO2 nanoparticulate hybrids

Author: François Ribot, Andrei Kanaev, Arseniy I. Kuznetsov, Laurence Rozes, A.P. Diaz-Gomez, Mamadou Kaba Traoré, Pavlo Gorbovyi, Boris N. Chichkov, Clément Sanchez, Luc Museur, Laboratoire d'Ingénierie des Matériaux et des Hautes Pressions (LIMHP), Centre National de la Recherche Scientifique (CNRS)-Institut Galilée-Université Paris 13 (UP13), Laboratoire des Sciences des Procédés et des Matériaux (LSPM), Université Paris 13 (UP13)-Institut Galilée-Université Sorbonne Paris Cité (USPC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Lasers (LPL), Université Paris 13 (UP13)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Novel Advanced Nano-Objects (LCMCP-NANO), and Laser Zentrum Hannover e.V. (LZH)
Subjects: Materials science, Mechanical Engineering, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Methacrylate, 01 natural sciences, 0104 chemical sciences, [SPI]Engineering Sciences [physics], Hydrolysis, Chemical engineering, Photoinduced charge separation, Polymerization, Mechanics of Materials, [CHIM]Chemical Sciences, Molecule, General Materials Science, Quantum efficiency, 0210 nano-technology, Hybrid material, ComputingMilieux_MISCELLANEOUS
Abstract: We report on a comparative study of photonic sensitivities of organic-inorganic hybrids prepared with size-selected 5 nm titanium-oxo-alkoxo nanoparticles and two different organic phases: HEMA (2-hydroxyethyl methacrylate) and MAPTMS (3-methacryloxypropyltrimethoxysilane). After organic polymerization, the obtained pHEMA-TiO2 and pMAPTMS-TiO2 hybrids are solids with different inter-component bindings. While surface exchange fixes organic (HEMA than pHEMA) groups on the nanoparticle surface, the titanium-oxo-alkoxo nanoparticles do not interact with the organic component in the pMAPTMS-TiO2 hydrid. Indeed, MAPTMS molecules are hydrolyzed forming condensed Si O Si species. The formation of Si O Ti bonds is observed at the organic thermal polymerization stage, which may be a signature of the silica layer formation at the particles surface. Consequently, the quantum efficiency of the photoinduced charge separation and storage in pMAPTMS-TiO2 hybrids is found considerably lower compared to that in pHEMA-TiO2 hybrids. The 3D micro-structuring of the hybrid solutions has been realized using 2-photon laser polymerization. The structures were mechanically more stable and easier to achieve in pMAPTMS-TiO2 compared to pHEMA-TiO2. Moreover, higher density of the photoinduced electrons decreases the damage threshold in the pHEMA-TiO2 hybrids.
Published: 2019

20. Denoising applied to spectroscopies – Part II: Decreasing computation time

Author: Christian Bonhomme, William Woelffel, Pierre-Aymeric Gilles, Guillaume Laurent, Emmanuelle Gouillart, Virgile Barret-Vivin, Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Surface du Verre et Interfaces (SVI), SAINT-GOBAIN-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), and The French Region Ile de France – SESAME program is acknowledged for financial support (700 MHz spectrometer).
Subjects: Signal processing, Noise reduction, Computation, 010401 analytical chemistry, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Singular Value Decomposition (SVD), 0104 chemical sciences, [INFO.INFO-PF]Computer Science [cs]/Performance [cs.PF], ComputingMethodologies_PATTERNRECOGNITION, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Singular value decomposition, benchmarking, Sensitivity (control systems), signal processing, 0210 nano-technology, [SPI.SIGNAL]Engineering Sciences [physics]/Signal and Image processing, Instrumentation, Algorithm, Cadzow denoising, Spectroscopy, Mathematics
Abstract: International audience; Spectroscopies are of fundamental importance but can suffer from low sensitivity. Singular Value Decomposition (SVD) is a highly interesting mathematical tool, which can be conjugated with low-rank approximation to denoise spectra andincrease sensitivity. SVD is also involved in data mining with Principal Component Analysis (PCA). In this paper, we focussed on the optimisation of SVD duration, which is a time-consuming computation. Both Intel processors (CPU) and Nvidia graphic cards (GPU) were benchmarked. A 100 times gain was achieved when combining divide and conquer algorithm, Intel Math Kernel Library (MKL), SSE3 (Streaming SIMD Extensions) hardware instructions and single precision. In such case, the CPU can outperform the GPU driven by CUDA technology. These results give a strong background to optimise SVD computation at the user scale.
Published: 2019

21. Electron Precise Sodium Carbaboride Nanocrystals from Molten Salts: Single Sources to Boron Carbides

Author: Gwenaëlle Rousse, Cristina Coelho-Diogo, Christel Gervais, Simon Delacroix, Fernando Igoa, Yann Le Godec, David Portehault, Yang Song, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Chimie du solide et de l'énergie (CSE), Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), HPC resources from GENCI-IDRIS (Grant 097535), and Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)
Subjects: Octahedral cluster, 010405 organic chemistry, chemistry.chemical_element, Nanoparticle, Crystal structure, Boron carbide, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, chemistry, X-ray photoelectron spectroscopy, Chemical engineering, Physical and Theoretical Chemistry, Boron, Powder diffraction, Solid solution
Abstract: International audience; Boron-rich solids exhibit specific crystal structures and unique properties, which are only very scarcely addressed in nanoparticles. In this work, we address the original inorganic structural chemistry and reactivity of boron-rich nanoparticles, by reporting the first occurrence of sodium carbaboride nanocrystals based on the NaB 5 C crystal structure. To design these sub-10 nm nano-objects, we use liquid-phase synthesis in molten salts at 900°C. By combining a set of characterization tools including powder Xray powder diffraction, transmission electron microscopy, solid-state nuclear magnetic resonance coupled to DFT modeling, and X-ray photoelectron spectroscopy, we demonstrate that these nanocrystals deviate from the ideal stoichiometry reported for the bulk compound. We suggest that the carbon and sodium contents compensate each other to ensure that the octahedral cluster-based framework is stabilized by fulfilling an electron counting rule. These nanocrystals encompass substituted octahedral covalent structural building units not reported in the related bulk compound. They then shed new light on the ability of nanoparticles to host wide solid solution ranges in covalent solids and then to yield new solids. We finally show that these nanocrystals are efficient single sources of boron and carbon to form a nanostructured boron carbide, thus paving the way to new nanostructured materials.
Published: 2021

22. Collagen suprafibrillar confinement drives the activity of acidic calcium-binding polymers on apatite mineralization

Author: Fabrice Soncin, Thierry Azaïs, Jean-Yves Sire, Camila B. Tovani, Jérémie Silvent, Marc Robin, Sidney Delgado, Marie-Madeleine Giraud-Guille, Yan Wang, Nadine Nassif, Capucine Sassoye, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Systématique, Evolution, Biodiversité (ISYEB ), Muséum national d'Histoire naturelle (MNHN)-École pratique des hautes études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université des Antilles (UA), Mécanismes de tumorigenèse et thérapies ciblées, Centre National de la Recherche Scientifique (CNRS)-Institut Pasteur de Lille, Réseau International des Instituts Pasteur (RIIP)-Réseau International des Instituts Pasteur (RIIP)-Université de Lille, Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Pasteur de Lille, Réseau International des Instituts Pasteur (RIIP)-Réseau International des Instituts Pasteur (RIIP)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), NASSIF, Nadine, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Muséum national d'Histoire naturelle (MNHN)-École Pratique des Hautes Études (EPHE), and Novel Advanced Nano-Objects (LCMCP-NANO)
Subjects: concentration, mineral, Polymers and Plastics, Polymers, [SDV]Life Sciences [q-bio], chemistry.chemical_element, Bioengineering, 02 engineering and technology, Calcium, Matrix (biology), 010402 general chemistry, 01 natural sciences, Apatite, Biomaterials, Extracellular matrix, biopolymer, Apatites, Materials Chemistry, Dentin, medicine, [CHIM]Chemical Sciences, [SDV.BBM.BC]Life Sciences [q-bio]/Biochemistry, Molecular Biology/Biochemistry [q-bio.BM], [SDV.BBM.BC] Life Sciences [q-bio]/Biochemistry, Molecular Biology/Biochemistry [q-bio.BM], Extracellular Matrix Proteins, Chemistry, Mineralization (soil science), self-assembly, 021001 nanoscience & nanotechnology, DMP1, 0104 chemical sciences, medicine.anatomical_structure, visual_art, confinement, visual_art.visual_art_medium, Biophysics, Collagen, 0210 nano-technology, Biomineralization
Abstract: International audience; Bone collagenous extracellular matrix provides a confined environment into which apatite crystals form. This biomineralization process is related to a cascade of events partly controlled by noncollagenous proteins. Although overlooked in bone models, concentration and physical environment influence their activities. Here, we show that collagen suprafibrillar confinement in bone comprising intra- and interfibrillar spaces drives the activity of biomimetic acidic calcium-binding polymers on apatite mineralization. The difference in mineralization between an entrapping dentin matrix protein-1 (DMP1) recombinant peptide (rpDMP1) and the synthetic polyaspartate validates the specificity of the 57-KD fragment of DMP1 in the regulation of mineralization, but strikingly without phosphorylation. We show that all the identified functions of rpDMP1 are dedicated to preclude pathological mineralization. Interestingly, transient apatite phases are only found using a high nonphysiological concentration of additives. The possibility to combine biomimetic concentration of both collagen and additives ensures specific chemical interactions and offers perspectives for understanding the role of bone components in mineralization.
Published: 2021

23. Synthesis in Molten Salts and Characterization of Li 6 B 18 (Li 2 O) x Nanoparticles

Author: Patrick Le Griel, David Portehault, Isabelle Génois, Christel Gervais, Yann Le Godec, Cristina Coelho-Diogo, Simon Delacroix, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and HPC resources from GENCI-IDRIS (Grant 097535)
Subjects: 010405 organic chemistry, Inorganic chemistry, chemistry.chemical_element, Nanoparticle, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, Characterization (materials science), Inorganic Chemistry, chemistry, [CHIM]Chemical Sciences, Lithium, Reactivity (chemistry), Physical and Theoretical Chemistry, Boron
Abstract: International audience; Lithium borides have been synthesized exclusively through classical solid-state chemistry processes that lead to bulk materials. Indeed, due to the lack of reactivity of the solid boron precursors usually employed and to the high covalent connectivity in such solids, high temperatures and long reaction times are necessary to obtain lithium borides. These conditions result in extensive crystal growth. Here we present the synthesis of nanoparticles of a lithium boride bearing tunnel-like cavities templated by neutral Li2O species, which have been reported to be labile. To reach this goal, a liquid-phase synthesis in inorganic molten salts has been developed. The Li6B18(Li2O)x nanoparticles have been characterized by scanning and transmission electronic microscopy (SEM and TEM), X-ray diffraction (XRD), and Raman spectroscopy. We provide an in-depth structural characterization by using 1H, 7Li, and 11B solid-state nuclear magnetic resonance (NMR) coupled with DFT modeling to provide the first assignment of 7Li and 11B solid-state NMR signals in lithium borides. We then assess the nanoparticle morphology oriented along the direction of the cavities. This feature shows similarities with structurally related hexagonal tungsten bronzes and could therefore affect the electrochemical and ion exchange properties.
Published: 2020

24. Homogeneous supported monolayer from microbial glycolipid biosurfactant

Author: Vincent Humblot, Niki Baccile, Cédric Boissière, Anyssa Derj, Ariane Deniset-Besseau, Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), 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), Laboratoire de Chimie Physique D'Orsay (LCPO), and Université Paris-Sud - Paris 11 (UP11)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: glycolipids, Materials science, microbial biosurfactants, supported lipid bilayers, dip-coating, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Dip-coating, biosurfactants, Colloid, Lamellar phase, Monolayer, Amphiphile, Materials Chemistry, microbial glycolipids, Lamellar structure, Physical and Theoretical Chemistry, [NLIN.NLIN-AO]Nonlinear Sciences [physics]/Adaptation and Self-Organizing Systems [nlin.AO], Spectroscopy, Substrate (chemistry), lamellar, [CHIM.MATE]Chemical Sciences/Material chemistry, Adhesion, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Chemical engineering, 0210 nano-technology
Abstract: International audience; The development of supported glycosylated lipid layers is an important trend in the field of glyconanomaterials for their interest in understanding sugar-sugar and protein-sugar interactions, these being at the core of cellular, bacterial or viral adhesion. The conventional self-assembled monolayer (SAM) approach generally requires a thiolated glycoconjugate and a gold substrate. In this work, we show how glycolipid amphiphiles of natural origin, commonly known as microbial biosurfactants, can be easily deposited onto a substrate. Spontaneously produced by microorganisms but lacking a thiol group, one can take advantage of their self-assembly properties to prepare homogeneous supported lipid monolayers (SLM). We then choose a saturated glucolipid, G-C18:0, which forms a colloidal lamellar phase under diluted conditions. The lamellae can then be deposited onto a substrate (silicon, gold) using a physical method (dip coating). Dip coating is preferred over more classical deposition methods (Langmuir-Blodgett-LB-, vesicle fusion or spin-coating) because of its versatility, compatibility with aqueous solutions and robust control of the thickness below 10 nm. Defect-free glycosylated SLM from a microbial biosurfactant are then easily developed. A combination of ellipsometry, fluorescence microscopy, atomic force microscopy and infrared nanospectroscopy (AFMIR) show that the glycosylated SLM are defect-free, have a thickness of 2.8 ± 1.0 nm and they are highly homogeneous at scales going from the nm to cm.
Published: 2022

25. Risk analysis and technology assessment of emerging (Gd,Ce)2O2S multifunctional nanoparticles: An attempt for early safer-by-design approach

Author: Anh-Minh Nguyen, Ana Elena Pradas del Real, Olivier Durupthy, Sophie Lanone, Corinne Chanéac, Sophie Carenco, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Mondor de Recherche Biomédicale (IMRB), Institut National de la Santé et de la Recherche Médicale (INSERM)-IFR10-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12), European Synchroton Radiation Facility [Grenoble] (ESRF), IMRB - GEIC2O/'Genetic and Environmental Interactions in COPD, Cystic fibrosis and Other (rare) respiratory diseases' [Créteil] (U955 Inserm - UPEC), Institut National de la Santé et de la Recherche Médicale (INSERM)-IFR10-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut National de la Santé et de la Recherche Médicale (INSERM)-IFR10-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12), and Gestionnaire, Hal Sorbonne Université
Subjects: [SDE] Environmental Sciences, murine macrophage RAW 264.7, General Chemical Engineering, ROS, Chemistry, cerium, oxysulfides, [SDE]Environmental Sciences, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, nanoparticles, lanthanides, safer-by-design, QD1-999
Abstract: Acceptability and relevance of nanoparticles in the society is greatly improved using a safer-by-design strategy. However, this is difficult to implement when too late in the development process or when nanoparticles are already on the market (e.g., TiO2). We employ this strategy for emerging nanoparticles of lanthanide oxysulfide of formula (Gd,Ce)2O2S, relevant for photocatalysis as well as for multimodal imaging, as the bandgap of the nanoparticles, related to their Ce content, impacts their ability to absorb visible light. As a first step, we investigated the production of reactive oxygen species (ROS) as a function of cerium content, in abiotic conditions and in vitro using murine macrophage RAW 264.7 cell line. We demonstrate that, at sub-lethal doses, Ce-containing oxysulfide nanoparticles are responsible for a higher ROS intracellular formation than cerium-free Gd2O2S nanoparticles, although no significant inflammatory response or oxidative stress was measured. Moreover, there was no significant loss of cerium as free cation from the nanoparticles, as evidenced by X-ray fluorescence mapping. Based on these results, we propose a risk analysis for lanthanide oxysulfide nanoparticles, leading to a technology assessment that fulfills the safer-by-design strategy.
Published: 2022

26. The shape and speciation of Ag nanoparticles drive their impacts on organisms in a lotic ecosystem

Author: Corinne Chanéac, Mélanie Auffan, Mark R. Wiesner, Bernard Angeletti, Jean-Yves Bottero, Lenka Brousset, Jérôme Rose, Alain Thiéry, E. Morel, Julien Issartel, Marie Tella, Clément Levard, Jean-Louis Hazemann, Catherine Santaella, Mohamed Barakat, Philippe Ortet, Centre européen de recherche et d'enseignement des géosciences de l'environnement (CEREGE), Institut de Recherche pour le Développement (IRD)-Aix Marseille Université (AMU)-Collège de France (CdF (institution))-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), Laboratoire d'Ecologie Microbienne de la Rhizosphère et d'Environnements Extrêmes (LEMIRE), Institut de Biosciences et Biotechnologies d'Aix-Marseille (ex-IBEB) (BIAM), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)-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)-Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)-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), Institut méditerranéen de biodiversité et d'écologie marine et continentale (IMBE), Avignon Université (AU)-Aix Marseille Université (AMU)-Institut de recherche pour le développement [IRD] : UMR237-Centre National de la Recherche Scientifique (CNRS), Analyses des eaux, sols et végétaux (US Analyses), Centre de Coopération Internationale en Recherche Agronomique pour le Développement (Cirad), Département Performances des systèmes de production et de transformation tropicaux (Cirad-PERSYST), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sorbonne Université (SU), Matériaux, Rayonnements, Structure (NEEL - MRS), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Duke University [Durham], Centre National de la Recherche Scientifique (CNRS)European Commission, ANR-10-NANO-0006,MESONNET,Utilisation de mésocosmes terrestres et aquatiques en réseau pour l'évaluation du risque associé à la dispersion de nanoparticules manufacturées(2010), European Project: 310584,EC:FP7:NMP,FP7-NMP-2012-LARGE-6,NANOREG(2013), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Collège de France (CdF (institution))-Institut national des sciences de l'Univers (INSU - CNRS)-Aix Marseille Université (AMU)-Institut National de la Recherche Agronomique (INRA), 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)-Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), and Matériaux, Rayonnements, Structure (MRS)
Subjects: nanomaterials [EN], River ecosystem, Materials Science (miscellaneous), media_common.quotation_subject, Argent, 010501 environmental sciences, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 01 natural sciences, Mesocosm, Plancton, 03 medical and health sciences, Milieu lotique, Water column, Ecosystem, ComputingMilieux_MISCELLANEOUS, 030304 developmental biology, 0105 earth and related environmental sciences, General Environmental Science, media_common, 0303 health sciences, Stress oxydatif, Impact sur l'environnement, [CHIM.MATE]Chemical Sciences/Material chemistry, Plankton, Bioaccumulation, [SDE.ES]Environmental Sciences/Environmental and Society, Speciation, 13. Climate action, Benthic zone, Environmental chemistry, M40 - Écologie aquatique, [SDE]Environmental Sciences, Environmental science, P02 - Pollution
Abstract: International audience; Silver nanomaterials with different shapes (spheres, plates, wires, rods, cubes) are valued by industries and scientists for their shape-dependent properties which make them useful for diverse applications. In a saferby-design perspective, controlling the shape of Ag nanomaterials could be an option to increase their properties while lowering either their hazard or their exposure potentials. Nine indoor aquatic mesocosms reproducing a lotic ecosystem were contaminated with chronic low-level additions of Ag nanospheres (Sp-Ag) and nanoplates (Pl-Ag) for a month. A shape-dependent impact under such environmentally relevant exposure conditions was observed. Pl-Ag induced a moderate oxidative stress in adult Gammarus fossarum (after molting) and a hormesis effect on planktonic microbial communities, while Sp-Ag had no effect. In an environmental risk perspective, our results highlight which ecological niches of a lotic ecosystem would be more impacted by Pl-Ag: (i) >72% of the total Ag was found fully sulfidized in surficial sediment and had only a moderate impact on benthic macro-organisms, (ii) only 11% to 15% of the Ag remained in the water column after 1 month, but Ag was under a more reactive speciation that impacts the planktonic community.
Published: 2020

27. Phase selective synthesis of nickel silicide nanocrystals in molten salts for electrocatalysis of the oxygen evolution reaction

Author: Ovidiu Ersen, Ram Kumar, Mounib Bahri, Christel Laberty-Robert, Cyril Thomas, Yang Song, David Portehault, Francisco Gonell, Clément Sanchez, Portehault, David, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and 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)
Subjects: [PHYS]Physics [physics], chemistry.chemical_classification, [CHIM.MATE] Chemical Sciences/Material chemistry, Materials science, Oxygen evolution, Intermetallic, chemistry.chemical_element, Salt (chemistry), [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrocatalyst, 01 natural sciences, [PHYS] Physics [physics], 0104 chemical sciences, Sodium silicide, chemistry.chemical_compound, Nickel, chemistry, Chemical engineering, General Materials Science, Iridium, 0210 nano-technology, Eutectic system
Abstract: International audience; We report phase selective synthesis of intermetallic nickel silicide nanocrystals in inorganic molten salts. NiSi and Ni2Si nanocrystals are obtained by reacting a nickel (II) salt and sodium silicide Na4Si4 in the molten LiI-KI inorganic eutectic salt mixture. We report that nickel silicide nanocrystals are precursors to active electrocatalysts in the oxygen evolution reaction (OER) and may be low-cost alternatives to iridium-based electrocatalysts.
Published: 2020

28. Chemical Heterogeneities within the Disordered Mineral domains of Aragonite Platelets in Nacre from the European Abalone Haliotis tuberculata

Author: Sylvain Huchette, Axel Gansmüller, Nadine Nassif, Guillaume Laurent, Widad Ajili, Nicolas Menguy, Stéphanie Auzoux-Bordenave, Thierry Azaïs, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF (institution))-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Cristallographie, Résonance Magnétique et Modélisations (CRM2), Centre National de la Recherche Scientifique (CNRS)-Université de Lorraine (UL), Scea France Haliotis, Biologie des Organismes et Ecosystèmes Aquatiques (BOREA), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-Muséum national d'Histoire naturelle (MNHN)-Institut de Recherche pour le Développement (IRD)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université des Antilles (UA), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université des Antilles (UA)-Muséum national d'Histoire naturelle (MNHN)-Institut de Recherche pour le Développement (IRD)-Sorbonne Université (SU)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011), and Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)
Subjects: food.ingredient, Abalone, 02 engineering and technology, engineering.material, 010402 general chemistry, 01 natural sciences, food, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, [CHIM]Chemical Sciences, Haliotis, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS, Mineral, biology, Chemistry, Aragonite, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, biology.organism_classification, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, Haliotis laevigata, Chemical engineering, engineering, 0210 nano-technology
Abstract: International audience; Since the observation in 2005 of a disordered mineral layer at the surface of aragonite platelets in abalone Haliotis laevigata nacre, the model of the organo–mineral interface in such biomineralized tissue has been challenged. As a direct interaction between the aragonite crystalline core and the organic matrix is no longer appropriate to describe such interface, a structural description of the disordered mineral domains at the atomic level is a key for a comprehensive view of nacre ultrastructure. Here, we use European abalone Haliotis tuberculata as a model to investigate aragonite nacre through high-resolution transmission electron microscopy (HR-TEM) and multinuclear solid state nuclear magnetic resonance (ssNMR). The presence of a disordered domain around aragonite crystals is shown through HR-TEM observations similarly to H. laevigata. The structure and the ionic composition of the disordered mineral environments of H. tuberculata nacre are investigated through 1H, 13C, 43Ca, and 23Na ssNMR. Interestingly, we demonstrate that the disordered mineral domains in nacre seem to be heterogeneous in terms of structure and chemical composition and do not match with amorphous calcium carbonate stricto sensu. At least three different carbonates species are evidenced, including CO32– and HCO3– present in the same mineral domain and closely associated with rigid H2O molecules. The local disorder around these ions is found to be inhomogeneous as some CO32– possess an aragonitic environment and are rather ordered (according to the position and line width of their 13C resonance) whereas, in opposition, the chemical environment around HCO3– is highly distributed. The analysis of potential cations as counterions revealed the presence of disordered Ca2+ and the presence of Na+ closely associated with HCO3–. On the basis of these structural data, we propose an atomic-level model for the disordered domains in abalone (H.tuberculata) nacre where the protonation level of carbonate ions, the proportion of sodium ions and the local disorder are increasing from the inner to the outer part of disordered domains. These results give an unprecedented structural view at the atomic scale of such disordered mineral domains in nacre aragonite tablets.
Published: 2020

29. Structure–Activity Relationship in Manganese Perovskite Oxide Nanocrystals from Molten Salts for Efficient Oxygen Reduction Reaction Electrocatalysis

Author: David Portehault, Vincent Vivier, Carlos M. Sánchez-Sánchez, Christel Laberty-Robert, Francisco Gonell, Christophe Méthivier, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Reactive Materials for Electrochemical Systems (LCMCP-RMES )
Subjects: Materials science, General Chemical Engineering, Oxide, Nanoparticle, chemistry.chemical_element, 02 engineering and technology, Manganese, 010402 general chemistry, Electrocatalyst, 01 natural sciences, 7. Clean energy, chemistry.chemical_compound, Materials Chemistry, Structure–activity relationship, Oxygen reduction reaction, [CHIM]Chemical Sciences, Perovskites, Redox reactions, Perovskite (structure), Oxides, General Chemistry, Transition metals, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, Nanocrystal, chemistry, Nanoparticles, 0210 nano-technology
Abstract: International audience; We report a synthesis pathway in molten salts toward ligand-free nanoparticles of the layered perovskite La0.5Sr1.5MnO4 (l-LSMO) and of the pseudocubic perovskite La0.7Sr0.3MnO3 (pc-LSMO). These particles are readily implemented as oxygen reduction reaction (ORR) electrocatalysts in alkaline conditions. They show high ORR selectivity for the 4-electron reduction of O2 in water. Among these two materials, pc-LSMO nanocrystals of 20 nm diameter exhibit high mass-normalized ORR activity for a perovskite material (21.4 A g–1oxide at 0.8 V/RHE) thanks to their relatively large surface area, high crystallinity, and electron mobility. These features provide pc-LSMO nanocrystals with remarkable stability compared to state-of-the-art perovskites, for instance, only a 5% increase of the overpotential at −0.05 mA cm–2oxide over 40 h. Thus, pc-LSMO nanocrystals are the most stable perovskite ORR electrocatalyst reported to date. This performance combined with high activity, high selectivity, and the absence of precious metals make La0.7Sr0.3MnO3 nanocrystals one of the best compromises for alkaline oxygen reduction reaction.
Published: 2020

30. Origin of transparency in scattering biomimetic collagen materials

Author: Flore Salviat, Milena Lama, Nadine Nassif, Clément Sanchez, Marco Faustini, Marc Robin, Jean-Marie Chassot, Rémi Carminati, Elodie Moulongui, Arnaud Bardouil, Mohamed Selmane, Yan Wang, Marie-Madeleine Giraud-Guille, Alba Marcellan, Elora Bessot, Chrystelle Salameh, Franck Artzner, Institut Européen des membranes (IEM), 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), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Laue-Langevin (ILL), ILL, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Sciences et Ingénierie de la Matière Molle (UMR 7615) (SIMM), 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)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Langevin - Ondes et Images (UMR7587) (IL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), ESPCI ParisTech, Ecole Nationale Supérieure de Chimie de Paris- Chimie ParisTech-PSL (ENSCP)-ESPCI ParisTech-Sorbonne Université (SU), Sciences et Ingénierie de la Matière Molle (SIMM), PSL Research University (PSL)-Sorbonne Université (SU)-ESPCI ParisTech-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: collagen, Materials science, [SDV]Life Sciences [q-bio], [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], Fibrillar Collagens, 02 engineering and technology, mechanical properties, 010402 general chemistry, 01 natural sciences, Light scattering, Photonic metamaterial, Cornea, Biomimetic Materials, Biomimetics, Phase (matter), Animals, Transparency (data compression), Microscale chemistry, Phase diagram, transparency, [PHYS]Physics [physics], [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Multidisciplinary, Scattering, self-assembly, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, photonic materials, 0104 chemical sciences, Order (biology), [CHIM.POLY]Chemical Sciences/Polymers, Chemical physics, Physical Sciences, [PHYS.PHYS.PHYS-MED-PH]Physics [physics]/Physics [physics]/Medical Physics [physics.med-ph], [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 0210 nano-technology
Abstract: International audience; Living tissues, heterogeneous at the microscale, usually scatter light. Strong scattering is responsible for the whiteness of bones, teeth, and brain and is known to limit severely the performances of biomedical optical imaging. Transparency is also found within collagen-based extracellular tissues such as decalcified ivory, fish scales, or cornea. However, its physical origin is still poorly understood. Here, we unveil the presence of a gap of transparency in scattering fibrillar collagen matrices within a narrow range of concentration in the phase diagram. This precholesteric phase presents a three-dimensional (3D) orientational order biomimetic of that in natural tissues. By quantitatively studying the relation between the 3D fibrillar network and the optical and mechanical properties of the macroscopic matrices, we show that transparency results from structural partial order inhibiting light scattering, while preserving mechanical stability, stiffness, and nonlinearity. The striking similarities between synthetic and natural materials provide insights for better understanding the occurring transparency.
Published: 2020

31. Unambiguous localization of titanium and iron cations in doped manganese hollandite nanowires

Author: María Hernando, David Portehault, Isabel Gómez-Recio, María Teresa Fernández-Díaz, Marina Parras, Clément Sanchez, Alberto Azor-Lafarga, M. Luisa Ruiz-González, José J. Calvino, José M. González-Calbet, Universidad Complutense de Madrid = Complutense University of Madrid [Madrid] (UCM), University of Cadiz, Institut Laue-Langevin (ILL), ILL, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, and Spanish National Centre for Electron Microscopy (CNME)
Subjects: Materials science, Neutron diffraction, Nanowire, chemistry.chemical_element, 02 engineering and technology, Manganese, 010402 general chemistry, 01 natural sciences, Catalysis, Nanomaterials, Hollandite, Materials Chemistry, Dopant, Metals and Alloys, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Crystallography, chemistry, Transmission electron microscopy, Ceramics and Composites, 0210 nano-technology, Titanium
Abstract: International audience; New insights into the chemical and structural features of iron or titanium-doped KxMnO2 hollandites are reported. Neutron diffraction and atomically resolved transmission electron microscopy elucidate the localization of the dopant cations that could be one of the key factors governing the functional activity of these nanomaterials.
Published: 2020

32. Following in Situ the Degradation of Mesoporous Silica in Biorelevant Conditions: At Last, a Good Comprehension of the Structure Influence

Author: Zeinab Chehadi, Corinne Chanéac, David Grosso, Omar Azzaroni, Clément Sanchez, Cédric Boissière, Pierre-Antoine Albouy, Marco Faustini, Andrea Cattoni, Elisa Bindini, Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Institut des Matériaux, de Microélectronique et des Nanosciences de Provence (IM2NP), Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas [La Plata] (INIFTA), Facultad de Ciencias Exactas [La Plata], Universidad Nacional de la Plata [Argentine] (UNLP)-Universidad Nacional de la Plata [Argentine] (UNLP), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS), and Novel Advanced Nano-Objects (LCMCP-NANO)
Subjects: In situ, Materials science, Nanoparticle, Nanotechnology, 02 engineering and technology, therapeutic vectors, 010402 general chemistry, 01 natural sciences, dissolution kinetic, Drug Delivery Systems, Ellipsometry, [CHIM]Chemical Sciences, Humans, General Materials Science, mesoporous silica, Porosity, Drug Carriers, High loading, Proteins, Mesoporous silica, 021001 nanoscience & nanotechnology, Silicon Dioxide, 0104 chemical sciences, Drug Liberation, Kinetics, Drug delivery, Degradation (geology), Nanoparticles, 0210 nano-technology, protein, ellipsometry
Abstract: International audience; Mesoporous silica nanoparticles (MSNs) have seen a fast development as drug delivery carriers thanks to their tunable porosity and high loading capacity. The employ of MSNs in biomedical applications requires a good understanding of their degradation behavior both to control drug release and to assess possible toxicity issues on human health. In this work, we study mesoporous silica degradation in biologically relevant conditions through in situ ellipsometry on model mesoporous nanoparticle or continuous thin films, in buffer solution and in media containing proteins. In order to shed light on the structure/dissolution relationship, we performed dissolution experiments far from soluble silicate species saturation. Via a complete decorrelation of dissolution and diffusion contributions, we proved unambiguously that surface area of silica vectors is the main parameter influencing dissolution kinetics, while thermal treatment and open mesoporous network architecture have a minor impact. As a logical consequence of our dissolution model, we proved that the dissolution lag-time can be promoted by selective blocking of the mesopores that limits the access to the mesoporous internal surface. This study was broadened by studying the impact of the organosilanes in the silica structure, of the presence of residual structuring agents, and of the chemical composition of the dissolution medium. The presence of albumin at blood concentration was found affecting drastically the dissolution kinetics of the mesoporous structure, acting as a diffusion barrier. Globally, we could identify the main factors affecting mesoporous silica materials degradation and proved that we can tune their structure and composition for adjusting dissolution kinetics in order to achieve efficient drug delivery.
Published: 2020

33. Aerosol synthesis of thermally stable porous noble metals and alloys by using bi-functional templates

Author: Mateusz Odziomek, Sophie Nowak, Mounib Bahri, Marco Faustini, Marion Giraud, Clément Sanchez, Cédric Tard, Benedikt Lassalle-Kaiser, Cédric Boissière, Jennifer Peron, Andrea Zitolo, Ovidiu Ersen, Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de photonique et de nanostructures (LPN), Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Synchrotron SOLEIL (SSOLEIL), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-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), Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Laboratoire de chimie moléculaire (LCM), École polytechnique (X)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace, Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-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))-Université de Strasbourg (UNISTRA), Novel Advanced Nano-Objects (LCMCP-NANO), Interfaces, Traitements, Organisation et Dynamique des Systèmes [Depuis 2020] (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure - Lyon (ENS Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Ecole Nationale Supérieure de Chimie de Paris- Chimie ParisTech-PSL (ENSCP)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SOLEIL), Dipartimento di Chimica, Università degli Studi di Roma 'La Sapienza' [Rome], Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace, Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Laboratoire de physique de la matière condensée (LPMC), Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), École supérieure du professorat et de l'éducation - Académie de Grenoble (ESPE Grenoble), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), 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), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Faustini, Marco, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: Nanostructure, Materials science, Absorption spectroscopy, Nanotechnology, 02 engineering and technology, engineering.material, 010402 general chemistry, Electrocatalyst, 01 natural sciences, Catalysis, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, Thermal stability, Electrical and Electronic Engineering, Porosity, Nanoscopic scale, [CHIM.MATE] Chemical Sciences/Material chemistry, Process Chemistry and Technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Mechanics of Materials, engineering, Noble metal, 0210 nano-technology
Abstract: International audience; Porous noble metal nanostructures providing high surface areas and large pore volumes are attractive for numerous applications especially catalysis. However, the synthesis of such architectures with nanoscale features is challenging because of i.e high surface energy. Previous reports are based on multi-step synthetic approaches with low yield thus not compatible with industrial scale. Herein, we demonstrate that hierarchical nanostructured noble metals and alloys, with thermal stability up to 800 °C, can be fabricated by a high throughput, green and straightforward aerosol-assisted synthesis using bi-functional reducing templates. We unravel the reduction mechanism at the solid/solid interface at the single-particle level using state-of-the-art techniques such as in situ Transmission Electron Microscopy, in situ synchrotron-based X-ray absorption spectroscopy. We propose a mechanism based on a radical process thermally triggered by the depolymerization of organic components. From a fundamental point of view, this study sheds light on the reduction processes of noble metals in the presence of organic compounds with important fundamental implications for catalysis and electrocatalysis.
Published: 2020

34. 31P MAS NMR and DFT study of crystalline phosphate matrices

Author: Thibault Charpentier, Karin Popa, Attila Kovács, Damien Bregiroux, Laura Martel, European Commission - Joint Research Centre [Karlsruhe] (JRC), Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Structure et Dynamique par Résonance Magnétique (LCF) (LSDRM), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: Nuclear and High Energy Physics, phosphates, Chemical substance, Materials science, Crystal structure, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, DFT calculations, 01 natural sciences, Divalent, chemistry.chemical_compound, Cluster (physics), cluster model, 31P NMR, Anisotropy, Instrumentation, chemistry.chemical_classification, Radiation, 010405 organic chemistry, Chemical shift, Isotropy, General Chemistry, Phosphate, 0104 chemical sciences, chemistry, Physical chemistry, Yavapaiite
Abstract: International audience; We present the study of the phosphorus local environment by using 31 P MAS NMR in a series of seven double monophosphates M II M IV (PO 4) 2 (M II and M IV being divalent and tetravalent cations, respectively) of yavapaiite and low-yavapaiite type crystal structures. Solid-state and cluster DFT calculations were found to be efficient for predicting the 31 P isotropic chemical shift and chemical shift anisotropy. To achieve this performance, however, a proper computational optimisation of the experimental structural data was required. From the three optimisation methods tested, the full optimisation provided the best reference structure for the calculation of the NMR parameters of the studied phosphates. Also, a better prediction of the chemical shifts was possible by using a correction to the GIPAW calculated shielding.
Published: 2020

35. Unraveling the Role of Alkali Cations in the Growth Mechanism of Gd2O2S Nanoparticles

Author: Andrea Gauzzi, Thi Kim-Chi Le, Anh-Minh Nguyen, Patrick Le Griel, Sophie Carenco, Clément Sanchez, David Carriere, Clément Larquet, Xavier Frogneux-Plé, Isabelle Génois, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011), ANR-16-CE09-0005,OxySUN,Nanomatériaux d'oxysulfures et oxynitrures pour l'électrocatalyse(2016), ANR-14-CE08-0003,DIAMONS,Phases denses intermédiaires liquides et amorphes comme modèle alternatif pour la synthèse de nanoparticules d'oxydes(2014), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)
Subjects: Lanthanide, Alkali ions, Chemistry, General Chemical Engineering, Organic solvent, Inorganic chemistry, Nanoparticle, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Alkali metal, 01 natural sciences, 0104 chemical sciences, Materials Chemistry, 0210 nano-technology, Mechanism (sociology), Colloidal synthesis
Abstract: International audience; Alkali cations are required for the colloidal synthesis of Ln$_2$O$_2$S nanoplates in organic solvent. Based on a thorough experimental analysis using various lanthanides and three alkali ions, we challenge the commonly accepted scenario of partial lanthanide substitution by the alkali, which is supposed to favor the sulfide insertion over the oxide one. Using SAXS-WAXS on aliquots taken from the synthesis medium, we demonstrate the formation of an alkali-stabilized oleate mesophase acting as a template for nanoparticles nucleation and growth. As a consequence, the alkali is not incorporated into the crystalline structure; nanoparticle growth requires only a low alkali concentration that can be readily washed away from the final nanoparticles powder. We expect that similar mesophases may form in other colloidal synthesis using oleates and small cations.
Published: 2020

36. Novel Hybrid Poly(L-lactic acid) from titanium oxo-cluster via reactive extrusion polymerization

Author: Gaelle Fontaine, Laurence Rozes, Séverine Bellayer, Fanny Bonnet, Elodie Louisy, Unité Matériaux et Transformations - UMR 8207 (UMET), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Centrale Lille Institut (CLIL), Université de Lille, CNRS, INRA, ENSCL, Unité Matériaux et Transformations - UMR 8207 [UMET], Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Institut National de la Recherche Agronomique (INRA)
Subjects: Materials science, Polymers and Plastics, Bulk polymerization, General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, Reactive extrusion, 010402 general chemistry, 01 natural sciences, Catalysis, Materials Chemistry, Hybrid poly(lactic acid), Ring Opening Polymerization, chemistry.chemical_classification, Molar mass, Organic Chemistry, Polymer, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, Polymerization, Oxo-clusters, 0210 nano-technology, Hybrid material, Titanium
Abstract: International audience; This paper reports the synthesis of novel hybrid poly(lactic acid) by use of a titanium oxo-cluster, acting both as a catalyst and crosslinking agent of the polymer matrix. The already reported oxo-cluster Ti16O16(OEt)32 ([Ti]16) was synthesized and screened at the lab-scale as catalyst for the bulk polymerization of L-lactide (L-LA). [Ti]16 was found to be highly active for this reaction as up to 90% conversion in 30 min was obtained, affording PLLAs with Mn up to 65 000 g·mol−1 and relatively narrow dispersities (1.2–1.6). These polymerization reactions were further transposed to reactive extrusion process in which [Ti]16 oxo-cluster kept its high activity, affording hybrid-PLLA materials with Mn close to 58 000 g·mol−1 (some PLLAs could not be dissolved). Electronic microprobe analysis of the resulting hybrid materials confirmed that the titanium oxo-cluster was well dispersed all over the PLLA matrix. Finally, it was shown that the hybrid PLLA containing [Ti]16 display superior dimensional stability under heat than commercial PLLA of same molar mass.
Published: 2020

37. Experimental Descriptors for the Synthesis of Multicationic Nickel Perovskite Nanoparticles for Oxygen Reduction

Author: Francisco Gonell, David Portehault, Vincent Vivier, Christel Laberty-Robert, Carlos M. Sánchez-Sánchez, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interfaces et Systèmes Electrochimiques (LISE), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Reactive Materials for Electrochemical Systems (LCMCP-RMES )
Subjects: Materials science, Synthesis methods, Nanoparticle, chemistry.chemical_element, nickel oxide, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Nanomaterials, Oxygen reduction reaction, General Materials Science, perovskite, Perovskite (structure), oxygen reduction reaction, Nickel oxide, molten salts, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Oxygen reduction, 0104 chemical sciences, Nickel, chemistry, Chemical engineering, layered materials, synthesis mechanism, 0210 nano-technology
Abstract: International audience; In many liquid-phase synthesis methods developed to produce nanomaterials, the key parameters governing the selective synthesis of solids and compounds are clearly identified, e.g. heat treatment profile, precursors solubility, pH, etc. Most of these well-understood approaches rely on relatively low temperature processes, below 400 °C, where conventional solvents are still stable. Interestingly, thermally stable inorganic molten salts enable to widen the temperature range for liquid-phase syntheses. They provide access to other families of crystalline solids requiring higher temperatures, as multicationic oxides. Nonetheless, the mechanisms that govern solid state formation and phase selection when different compounds compete are poorly understood. Herein, we report how experimental parameters, such as temperature, time, reaction medium composition and solvent oxo-basicity, enable to drive the synthesis mechanisms in molten salts towards nanoscaled multicationic oxides. We especially enlighten the phase-selective synthesis of pseudo-cubic perovskite LaNiO3 and layered Ruddlesden-Popper phases La2NiO4 and LaSrNiO4 at the nanoscale, by suggesting that the oxidation state of the metallic precursor plays a key role in the reaction pathway. This allows designing electrocatalysts for oxygen reduction reaction.
Published: 2020

38. Insights for OCP Identification and Quantification in the Context of Apatite Biomineralization

Author: Stanislas Von Euw, Jean-Marc Krafft, Thierry Azaïs, Marc Robin, Sandrine Gomes, Guillaume Renaudin, Nadine Nassif, Guylène Costentin, Littoral, Environnement, Télédétection, Géomatique (LETG - Nantes), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École pratique des hautes études (EPHE)-Université de Brest (UBO)-Université de Rennes 2 (UR2), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)-Institut de Géographie et d'Aménagement (IGARUN), Université de Nantes (UN)-Université de Nantes (UN), Institut de Chimie de Clermont-Ferrand (ICCF), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC), Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI) (LCMCP (site Paris VI)), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Ecole Nationale Supérieure de Chimie de Paris- Chimie ParisTech-PSL (ENSCP)-Centre National de la Recherche Scientifique (CNRS), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011)
Subjects: carbonated apatite, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Apatite, in situ Raman, chemistry.chemical_compound, symbols.namesake, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, [CHIM]Chemical Sciences, General Materials Science, Amorphous calcium phosphate, Octacalcium phosphate, ComputingMilieux_MISCELLANEOUS, solid state NMR, Chemistry, Rietveld refinement, General Chemistry, Nuclear magnetic resonance spectroscopy, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Chemical engineering, Solid-state nuclear magnetic resonance, visual_art, symbols, visual_art.visual_art_medium, OCP, Carbonate, precursors, 0210 nano-technology, Raman spectroscopy, Biomineralization
Abstract: International audience; Calcium phosphates (CaPs) are one of the major mineral families of wide interest in biomineralization and biomaterial development. The identification and quantification of the different CaP phases (crystalline and amorphous) remains a major challenge in both in vitro and in vivo systems. This work aims to provide critical analysis of the different analytical techniques, Raman spectroscopy, solid-state NMR spectroscopy (ssNMR) and X-ray diffraction (XRD), which are used for the discrimination of octacalcium phosphate (OCP) from hydroxyapatite (HAp). Low amounts of OCP (∼10 wt%) can be detected by Raman spectroscopy in the presence of biomimetic carbonated apatite (cHAp), provided that the ν(HPO4) contribution with weak intensity from OCP at 1008 cm−1 is observable or that the spectral decomposition of the overlapped ν1(PO4) bands from OCP and cHAp is performed. However, Raman is not suitable for quantification purposes. In contrast, the quantification of OCP in proportions down to 10 wt% is easily performed with 31P solid state NMR. Opposite to solid state NMR, Raman can be implemented under in situ conditions to monitor the time dependence of the biomineralization process without any sampling perturbation. An approach combining the advantages of in situ micro-Raman spectroscopy and the sensitivity of ex situ solid state NMR was used to monitor the formation of biomimetic carbonated apatite from an acidic aqueous solution of phosphate, carbonate and calcium ions. In relation with the progressive increase of pH, we identify the transient phases, the precursors of cHAp: it is shown that an amorphous calcium phosphate phase (ACP) is first formed and subsequently transforms into OCP that then progressively turns into cHAp. Finally, powder X-ray diffraction coupled to Rietveld refinement was found to be very powerful in quantifying very small amounts of residual OCP in cHAp (down to 2 wt%). Upon the OCP transformation into cHAp, the decrease of the relative intensity of the (100) diffraction peak of the transient OCP phase was ascribed to an alteration of its hydrated layers, related to incorporation of water molecules and/or carbonate anions with reaction time. Such carbonate uptake in the course of transformation of OCP into cHAp could explain the origin of carbonate substitutions in the final biomimetic carbonated apatite.
Published: 2020

39. Modified Synthesis Strategies for the Stabilization of low n Tin O2n-1 Magnéli Phases

Author: Clément Sanchez, David Portehault, Luisa Ruiz-González, Marina Parras, Alberto Azor-Lafarga, José M. González-Calbet, Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, General Chemical Engineering, Superlattice, chemistry.chemical_element, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biochemistry, Metal, Transition metal, Materials Chemistry, ComputingMilieux_MISCELLANEOUS, Sol-gel, Electron energy loss spectroscopy, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Chemical physics, visual_art, visual_art.visual_art_medium, 0210 nano-technology, Tin, Titanium
Abstract: Titanium reduced oxides TiO2-x occupy, since long time, a prominent place on the landscape of binary metal oxides because of their intriguing ability to form extended defects that affect both the formation of new superlattices and different electronic behaviours. Related to these features, a wide range of practical applications has been achieved. Moved by the conviction of the great potential of understanding the influence of the reactivity, compositional variations and size effects on their functional properties, the aim of this personal account is the optimization of a recently developed strategy for the stabilization of low n Tin O2n-1 terms. In particular, we will focus on the Ti4 O7 composition as well as the incorporation of transition metals, like Mn, in order to deal with new reduced Magneli phases.
Published: 2018

40. Multicationic Sr4Mn3O10 mesostructures: molten salt synthesis, analytical electron microscopy study and reactivity

Author: Irma N. González-Jiménez, Juan C. Hernández-Garrido, Christel Laberty-Robert, David Portehault, Clément Sanchez, Miguel López-Haro, Almudena Torres-Pardo, José M. González-Calbet, Marina Parras, Simon Rano, José J. Calvino, Aurea Varela, Universidad Complutense de Madrid = Complutense University of Madrid [Madrid] (UCM), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Universidad de Cádiz (UCA), and Novel Advanced Nano-Objects (LCMCP-NANO)
Subjects: Materials science, Nanostructure, Process Chemistry and Technology, Electron energy loss spectroscopy, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Surface energy, 0104 chemical sciences, chemistry.chemical_compound, Electron tomography, chemistry, Chemical engineering, Mechanics of Materials, Transmission electron microscopy, Strontium hydroxide, General Materials Science, Surface charge, Electrical and Electronic Engineering, Molten salt, 0210 nano-technology
Abstract: International audience; Inorganic molten salts are known as fluxes for the synthesis of novel bulk inorganic compounds and of mesostructures and nanostructures with crystal habits different from those observed in more conventional solvents. However, they have not demonstrated the ability to provide mesostructures and nanostructures of complex metal oxides that are currently unreported at the mesoscale and nanoscale. In this report, we show the first occurrence of Sr4Mn3O10 at the mesoscale, as platelets synthesized in molten strontium hydroxide at 600 °C with basal faces of few hundreds of nanometers and thicknesses ranging from 20 to 100 nm. We address carefully the atom-scale structure by transmission electron microscopy, including electron energy loss spectroscopy and electron tomography. We then propose that the final morphology is driven by the surface charge of each facet through surface energy. The reactivity of these platelets is then addressed, highlighting cation leaching when in contact with acidic water, which results in crystalline–amorphous core–shell platelets that are active electrocatalysts towards the oxygen reduction reaction.
Published: 2018

41. Aerosol processing: a wind of innovation in the field of advanced heterogeneous catalysts

Author: Damien P. Debecker, Alexandra Chaumonnot, Solène Le Bras, Clément Sanchez, Cédric Boissière, Université Catholique de Louvain = Catholic University of Louvain (UCL), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), IFP Energies nouvelles (IFPEN), and Chaire Chimie des matériaux hybrides
Subjects: Materials science, Nanoparticle, Nanotechnology, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Catalysis, Nanomaterials, Aerosol, Suspension (chemistry), Methanation, Spray drying, [CHIM]Chemical Sciences, 0210 nano-technology, Porosity
Abstract: International audience; Aerosol processing is long known and implemented industrially to obtain various types of divided materials and nanomaterials. The atomisation of a liquid solution or suspension produces a mist of aerosol droplets which can then be transformed via a diversity of processes including spray-drying, spray pyrolysis, flame spray pyrolysis, thermal decomposition, micronisation, gas atomisation, etc. The attractive technical features of these aerosol processes make them highly interesting for the continuous, large scale, and tailored production of heterogeneous catalysts. Indeed, during aerosol processing, each liquid droplet undergoes well-controlled physical and chemical transformations, allowing for example to dry and aggregate pre-existing solid particles or to synthesise new micro- or nanoparticles from mixtures of molecular or colloidal precursors. In the last two decades, more advanced reactive aerosol processes have emerged as innovative means to synthesise tailored-made nanomaterials with tunable surface properties, textures, compositions, etc. In particular, the “aerosol-assisted sol–gel” process (AASG) has demonstrated tremendous potential for the preparation of high-performance heterogeneous catalysts. The method is mainly based on the low-cost, scalable, and environmentally benign sol–gel chemistry process, often coupled with the evaporation-induced self-assembly (EISA) concept. It allows producing micronic or submicronic, inorganic or hybrid organic–inorganic particles bearing tuneable and calibrated porous structures at different scales. In addition, pre-formed nanoparticles can be easily incorporated or formed in a “one-pot” bottom-up approach within the porous inorganic or hybrid spheres produced by such spray drying method. Thus, multifunctional catalysts with tailored catalytic activities can be prepared in a relatively simple way. This account is an overview of aerosol processed heterogeneous catalysts which demonstrated interesting performance in various relevant chemical reactions like isomerisation, hydrogenation, olefin metathesis, pollutant total oxidation, selective oxidation, CO2 methanation, etc. A short survey of patents and industrial applications is also presented. Our objective is to demonstrate the tremendous possibilities offered by the coupling between bottom up synthesis routes and these aerosol processing technologies which will most probably represent a major route of innovation in the mushrooming field of catalyst preparation research.
Published: 2018

42. Shedding Light on Functional Hybrid Nanocomposites 19th Century Paint Medium

Author: Ovidiu Ersen, Frédéric Gobeaux, Dris Ihiawakrim, Maguy Jaber, Marco Faustini, Cristina Coelho-Diogo, Christel Gervais, Philippe Walter, Hélène Pasco, Clément Sanchez, Laurence de Viguerie, Laboratoire d'Archéologie Moléculaire et Structurale (LAMS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut d’Etudes Avancées de l’Université de Strasbourg - Institute for Advanced Study (USIAS), Université de Strasbourg (UNISTRA), ANR-10-LABX-0068,MiChem,Multi-Scale Integrative Chemistry : From Single Molecule to Nano-edifices(2010), Palacin, Serge, Multi-Scale Integrative Chemistry : From Single Molecule to Nano-edifices - - MiChem2010 - ANR-10-LABX-0068 - LABX - VALID, Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), University of Strasbourg Institute of Advanced Study (USIAS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique
Subjects: [CHIM.MATE] Chemical Sciences/Material chemistry, Nanocomposite, Materials science, 010405 organic chemistry, Mastic Resin, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Biomaterials, Hybrid system, Electrochemistry, Hybrid material, Lead oxide
Abstract: International audience; British 19th century painters formulated gelled systems often described as ideal paint mediums. These so-called megilps or gumtions are based on common paint materials like linseed oil, lead acetate, and mastic resin, and allowed painters such as J.M.W Turner to improve their paint's properties and achieve unprecedented effects in an age of innovation. To propose a structural scheme of these hybrid systems of unprecedented complexity, it is paramount to design and study model systems using a broad combination of advanced spectroscopic techniques and microscopies. Through this approach, gel Mediums can be described as nanocomposites based on lead metallogels co-existing with lead oxide nanoparticles and a partially polymerized fraction. These functional hybrid materials created a real breakthrough on 19th century paints performances.
Published: 2021

43. Hollow Iridium-Based Catalysts for the Oxygen Evolution Reaction in Proton Exchange Membrane Water Electrolyzers

Author: Jacques Rozière, Cédric Boissière, Deborah J. Jones, Jennifer Peron, Cédric Tard, Marco Faustini, Marion Giraud, Interfaces, Traitements, Organisation et Dynamique des Systèmes (ITODYS (UMR_7086)), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Electrochimie Moléculaire (LEM (UMR_7591)), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Université Paris Diderot - Paris 7 (UPD7)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and 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)
Subjects: Aqueous solution, Chemistry, Inorganic chemistry, Oxygen evolution, Proton exchange membrane fuel cell, chemistry.chemical_element, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Thermal treatment, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Catalysis, law.invention, law, Iridium, Crystallization, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract: The performance of Proton Exchange Membrane Electrolyzers (PEMWE) is mostly impeded by the efficiency of the anode catalysts allowing for the Oxygen Evolution Reaction (OER) to occur. New catalytic materials should possess at least as high performance and stability as state of the art materials, since the price of electrolysis is mostly impacted by the price of electricity and higher overpotentials would render the catalysts not viable for application in PEMWE. The use of noble metal at the anode for the OER is at the current stage essential due to the highly oxidative and strongly acidic environment. Nevertheless, due to cost and resources considerations, it is necessary to reduce the noble metal content. In addition, according to present industrial requirements, PEMWE cells should be able to work at very high current density and under high pressure. Water and gases management are also a major challenge in PEMWE catalyst layers, and unlike in fuel cells or PEMWE cathodes the use of a cheap carbon based porous support for electronic conduction at the anode is highly undesirable due to highly anodic potential. We have developed a cheap, clean and easily scalable synthesis method to produce highly porous iridium-based materials. The materials are synthesized in aqueous solutions in presence of a porogen. The resulting material is further calcinated to remove the porogen and initiate crystallization of the inorganic phase. By adjusting reactant concentrations and calcination conditions, metallic iridium, iridium oxide or mixed oxides can be obtained. This last point is of high importance since in addition to reducing noble metals content compared to current technologies, the atomic neighborhood of dissimilar metals is expected to modify the monometallic behavior and potentially gives rise to new desired characteristics, i.e.to decrease the OER overpotential and/or increase the material stability. Structural characteristics and chemical composition of the materials have been determined using XRD, XPS and XRF. The influence of the thermal treatment has a strong impact on the crystallite size and the composition of the particle surface. SEM-FEG and BET characterizations have shown that the type of the porogen used for material synthesis directly impacts its morphology and porosity. To assess the catalytic performances of these hierarchically porous materials, a screening of the electrocatalytic activity of a series of prepared materials has been performed using a three-electrodes electrochemical setup. The optimized material shows lower overpotential than commercial Ir or IrO2 nanoparticles as shown on the figure thereafter. Finally, selected materials have been used to prepare anode catalyst layers and have been tested in a complete electrolysis device. With a loading of 2 mg cm-2 in Iridium, a potential of 1.65 V at 1 A cm-2 and of 1.85 V at 2 A cm-2 is obtained. The produced specific morphologies are very well adapted to the formation of porous percolating networks, which promote gases and water transport throughout the catalyst layer. Figure 1
Published: 2017

44. Interfacial Mechanisms of Water Vapor Sorption into Cellulose Nanofibril Films as Revealed by Quantitative Models

Author: Marco Faustini, Tekla Tammelin, Minna Hakalahti, Cédric Boissière, Eero Kontturi, VTT Technical Research Centre of Finland (VTT), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Aalto University
Subjects: Langmuir, Materials science, ADSORPTION, Polymers and Plastics, SURFACE, FEATURES, Nanofibers, Analytical chemistry, Bioengineering, 02 engineering and technology, 010402 general chemistry, ISOTHERM, 01 natural sciences, Biomaterials, Adsorption, Piperidines, QUARTZ-CRYSTAL MICROBALANCE, Materials Chemistry, Cellulose, Oxidized, Relative humidity, ta216, ta116, ComputingMilieux_MISCELLANEOUS, ELLIPSOMETRY, ta1182, Humidity, Sorption, Quartz crystal microbalance, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, BET, TRANSPORT, 0104 chemical sciences, Steam, NANOCRYSTALS, Absorption, Physicochemical, Absorption (chemistry), POLYMERS, 0210 nano-technology, Water vapor
Abstract: Humidity is an efficient instrument for facilitating changes in local architectures of two-dimensional surfaces assembled from nanoscaled biomaterials. Here, complementary surface-sensitive methods are used to collect explicit and precise experimental evidence on the water vapor sorption into (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) oxidized cellulose nanofibril (CNF) thin film over the relative humidity (RH) range from 0 to 97%. Changes in thickness and mass of the film due to water vapor uptake are tracked using spectroscopic ellipsometry and quartz crystal microbalance with dissipation monitoring, respectively. Experimental data is evaluated by the quantitative Langmuir/Flory-Huggins/clustering model and the Brunauer-Emmett-Teller model. The isotherms coupled with the quantitative models unveil distinct regions of predominant sorption modes: specific sorption of water molecules below 10% RH, multilayer build-up between 10 to 75% RH, and clustering of water molecules above 75% RH. The study reveals the sorption mechanisms underlying the well-known water uptake behavior of TEMPO oxidized CNF directly at the gas-solid interface.
Published: 2017

45. Surface-induced assembly of sophorolipids

Author: Ahmed Hamraoui, Niki Baccile, Vincent Humblot, Jessie Peyre, Marco Faustini, Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé ( SMiLES ), Laboratoire de Chimie de la Matière Condensée de Paris ( LCMCP ), Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Collège de France ( CdF ) -Centre National de la Recherche Scientifique ( CNRS ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ) -Collège de France ( CdF ) -Centre National de la Recherche Scientifique ( CNRS ), Matériaux et Biologie ( MATBIO ), Université Paris Descartes - Faculté des Sciences Fondamentales et Biomédicales ( UPD5 Sciences ), Université Paris Descartes - Paris 5 ( UPD5 ), Matériaux Hybrides et Nanomatériaux ( MHN ), Laboratoire de Réactivité de Surface ( LRS ), Centre National de la Recherche Scientifique ( CNRS ) -Université Pierre et Marie Curie - Paris 6 ( UPMC ), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (SMiLES), 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)-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), Matériaux et Biologie (MATBIO), Université Paris Descartes - Faculté des Sciences Fondamentales et Biomédicales (UPD5 Sciences), Université Paris Descartes - Paris 5 (UPD5), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Collège de France (CdF)-Centre National de la Recherche Scientifique (CNRS), Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC), Matériaux Hybrides et Procédés (LCMCP-MHP ), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP)
Subjects: Anatase, Materials science, Silicon, Scanning electron microscope, Sophorolipid, General Physics and Astronomy, chemistry.chemical_element, Electron donor, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Micelle, Surface energy, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry.chemical_compound, Chemical engineering, chemistry, [ CHIM.THEO ] Chemical Sciences/Theoretical and/or physical chemistry, Organic chemistry, Relative humidity, Physical and Theoretical Chemistry, 0210 nano-technology
Abstract: International audience; The surface self-assembly properties of acidic sophorolipids, a bolaform microbial glycolipids with pH-responsive properties in solution, were studied based on the chemical nature of the support and pH of the solution. Sophorolipids generally form micelles in water but formation of morphologies like platelets and twisted fibers depending on pH have also been reported. The surface self-assembly was achieved using dip-coating on three different substrates namely gold, silicon(111) and TiO 2 anatase. Deposition conditions (dip-coating withdrawal speed, relative humidity, temperature) were tested, and it was found that optimum self-assembly occurred at a withdrawal speed of 1 mm s À1 , T of 25 1C and relative humidity of 25%. The local structure of the sophorolipid films was characterized by Atomic Force Microscopy, while Scanning Electron Microscopy was used to characterize the spatial homogeneity. We also attempted to correlate dispersive, electron donor and electron attractor surface energy components, using Good–Van Oss's approach, and the behavior of sophorolipids. We found that when the surface energy is dominated by dispersive components, sophorolipids spontaneously assemble into entangled needles at all pH values (4, 6 and 11). However, when the surface energy is dominated by electronic components, pH has a strong influence on the surface self-assembly. We could discriminate three major organizations: homogeneous layer, isolated aggregates and a two-dimensional network similar to block copolymer surface self-assembly.
Published: 2017

46. A pure aqueous route to mesoporous silica thin films via dip-coating of prefabricated hybrid micelles

Author: Heiko Zschiedrich, Cédric Boissière, Patricia J. Kooyman, Eric Prouzet, Institut Européen des membranes (IEM), 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), DelftChemTech/NCH REM, Delft University of Technology (TU Delft), Institute for Nanotechnology [Waterloo], University of Waterloo [Waterloo], Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Dip-coating, Nanostructure, Materials science, Evaporation-induced self-assembly, Mesoporous, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Micelle, Biomaterials, Materials Chemistry, Composite material, Aqueous solution, Ellipsoporosimetry, Silica, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Mesoporous silica, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Evaporation (deposition), 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Mesoporous organosilica, Thin ﬁlm, Ceramics and Composites, 0210 nano-technology, Mesoporous material
Abstract: Mesoporous thin films were prepared by dip-coating with a purely aqueous method, as a substitute for the alcohol-based evaporation-induced self-assembly route. Unlike other aqueous routes that require a very slow pulling rate possible only using high performance dip-coaters, as a result of the high surface tension of water, this new process works with standard dip-coaters and at similar pulling rates as are used for the evaporation-induced self-assembly route. This unique asset is the result of the synthesis of prefabricated self-assembled silicate/organic hybrid micelles. These building blocks are concentrated before use, which provides a gelling edge after moderate evaporation. As a result, defect-free continuous mesoporous films with well-organized hexagonally packed pores were prepared after optimization of both the evaporation rate of the solution of hybrid micelles and the dip-coater pulling rate. The transmission electron microscopy observation reveals the hexagonally packed structure of mesoporous silica film. This nanostructure has already been observed on films prepared with the evaporation-induced self-assembly process, but it is the first time it is obtained with a pure aqueous method, based on prefabricated hybrid micelles, not on controlled evaporation of mesophases.
Published: 2016

47. Morphological and Structural Evolution of Co3O4 Nanoparticles Revealed by in Situ Electrochemical Transmission Electron Microscopy during Electrocatalytic Water Oxidation

Author: Nathaly Ortiz Peña, Christel Laberty-Robert, David Portehault, Sophie Carenco, Ovidiu Ersen, Clément Sanchez, Dris Ihiawakrim, Benedikt Lassalle-Kaiser, Madeleine Han, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-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), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Agence Nationale de la Recherche ANR, ANR-16-CE05-0011,InSiChem,Etude ' in-situ ' et multiéchelle d'électrocatalyseurs pour la conversion d'énergie(2016), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique
Subjects: In situ, Materials science, General Engineering, Oxygen evolution, General Physics and Astronomy, Nanoparticle, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, Electrocatalyst, 01 natural sciences, 7. Clean energy, Structural evolution, 0104 chemical sciences, Chemical engineering, Transmission electron microscopy, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, General Materials Science, 0210 nano-technology, Cobalt oxide, ComputingMilieux_MISCELLANEOUS
Abstract: Unveiling the mechanism of electrocatalytic processes is fundamental for the search of more efficient and stable electrode materials for clean energy conversion devices. Although several in situ te...
Published: 2019

48. Stability and degradation of PEO20PPO70PEO20 triblock copolymers in mesostructured silica

Author: Sandra Casale, Bénédicte Lebeau, Brindusa Dragoi, François Ribot, Guillaume Laurent, Anne Davidson, Mohamed Selmane, David Kreher, Taissire Benamor, Cédric Boissière, Patrick Schmidt, Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Alexandru Ioan Cuza University of Iași [Romania], Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-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), Centre de Biotechnologie de Borj Cédria (Hammam-Lif, Tunisie), Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Novel Advanced Nano-Objects (LCMCP-NANO), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Eberhard Karls Universität Tübingen = Eberhard Karls University of Tuebingen, Chimie des polymères (LCP), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut Parisien de Chimie Moléculaire (IPCM), Chimie Moléculaire de Paris Centre (FR 2769), École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-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)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Paris-Ile-de-France - SESAME program (700 MHz spectrometer), PERFORM-ERA ‘‘Post- doctoral Performance for Integration in the European Research Area’’ (ID-57649), financed by the European Social Fund and the Romanian Government, Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), 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), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Chimie Moléculaire de Paris Centre (FR 2769), and Laurent, Guillaume
Subjects: [CHIM.POLY] Chemical Sciences/Polymers, Materials science, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Biomaterials, Hydrolysis, chemistry.chemical_compound, Materials Chemistry, Copolymer, Propylene oxide, ordered, P123, structured, [CHIM.MATE] Chemical Sciences/Material chemistry, Ethylene oxide, Precipitation (chemistry), technology, industry, and agriculture, template, General Chemistry, NIR, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Decomposition, NMR, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, Spray drying, Ceramics and Composites, Self-assembly, 0210 nano-technology
Abstract: International audience; Organic−inorganic hybrid mesostructured silicas are prepared, without stirring (at pH = 0.0) and with stirring (at pH = 0.6) to obtain isolated and gyroidal-like attached silica grains with incorporated triblock P123 poly (ethylene oxide)-poly (propylene oxide)–poly (ethylene oxide) copolymers. Selected hybrids are submitted to various thermal and aging treatments for studying hydrolysis and oxidation of PEO and PPO chains. Two complementary spectroscopic techniques are used: near-infrared (NIR) with measurements performed in diffuse reflectance, as well as 1H and 13C liquid- and solid-state nuclear magnetic resonance (NMR) to study the mobility and stability of PEO and PPO chains. With precipitated fresh hybrids, the ratio of PEO over (PEO + PPO) units is lower (30% ± 5%) than in theory. This ratio also decreases depending on temperature when a hydrothermal treatment is applied. An acidic hydrolysis involving both PEO and PPO chains, with generated fragments eliminated by washing with water and/or synthesis liquor, is then demonstrated. For comparison, another hybrid obtained by spray drying via evaporation-induced self assembly mechanism is also studied. Its NMR signals are much more stable than those of the samples prepared by precipitation. Depending on aging time, thermal history, and materials processing, the textural properties and template decomposition inside mesostructured silica are found significantly different. The influence of the hydrolysis and oxidation of the template onto final materials texture is likely to be as important as the processing conditions.
Published: 2019

49. High-Pressure Melting Curve of Zintl Sodium Silicide Na4Si4 by In Situ Electrical Measurements

Author: Ram Kumar, Cristina Coelho-Diogo, David Portehault, H. Moutaabbid, Alexandre Courac, Carlos Renero-Lecuna, Yann Le Godec, Christel Gervais, Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), French Région Ile de France - SESAME, ANR-17-ERC2-0032,MOLTEN,Mélanges de sels fondus vers des nanomatériaux avancés(2017), and ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011)
Subjects: Work (thermodynamics), 010405 organic chemistry, Analytical chemistry, Ionic bonding, Conductance, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Melting curve analysis, 0104 chemical sciences, Ion, Inorganic Chemistry, Sodium silicide, chemistry.chemical_compound, chemistry, Melting point, Electrical measurements, Physical and Theoretical Chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Abstract: International audience; The inorganic chemistry of the Na–Si system at high pressure is fascinating, with a large number of interesting compounds accessible in the industrial pressure scale, below 10 GPa. In particular, Na4Si4 is stable in this whole pressure range and thus plays an important role in understanding the thermodynamics and kinetics underlying materials synthesis at high pressures and high temperatures. In the present work, the melting curve of the Zintl compound Na4Si4 made of Na+ and Si44– tetrahedral cluster ions is studied at high pressures up to 5 GPa, by using in situ electrical measurements. During melting, the insulating Na4Si4 solid transforms into an ionic conductive liquid that can be probed through the conductance of the whole high-pressure cell, i.e., the system constituted of the sample, the heater, and the high-pressure assembly. Na4Si4 melts congruently in the studied pressure range, and its melting point increases with pressure with a positive slope dTm/dp of 20(4) K/GPa.
Published: 2019

50. Formation of stable strontium-rich amorphous calcium phosphate: Possible effects on bone mineral

Author: Alexandre Gloter, Mohamed Selmane, Camila B. Tovani, Nadine Nassif, Thierry Azaïs, Ana Paula Ramos, Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des matériaux de Paris-Centre (IMPC), Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Centre of Marine Sciences [Faro] (CCMAR), University of Algarve [Portugal], Matériaux Hybrides et Procédés (LCMCP-MHP ), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP)
Subjects: inorganic chemicals, Calcium Phosphates, 0206 medical engineering, Osteoporosis, Biomedical Engineering, chemistry.chemical_element, 02 engineering and technology, Biochemistry, Bone and Bones, Bone remodeling, Biomaterials, X-Ray Diffraction, Biomimetic Materials, medicine, Dentin, Amorphous calcium phosphate, Molecular Biology, Bone mineral, Strontium, Minerals, Chemistry, OSSO E OSSOS, General Medicine, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, medicine.disease, Tooth enamel, 020601 biomedical engineering, medicine.anatomical_structure, Durapatite, Biophysics, Calcium, 0210 nano-technology, Crystallization, Biotechnology, Biomineralization
Abstract: International audience; Bone, tooth enamel, and dentin accumulate Sr 2+ , a natural trace element in the human body. Sr 2+ comes from dietary and environmental sources and is thought to play a key role in osteoporosis treatments. However, the underlying impacts of Sr 2+ on bone mineralization remain unclear and the use of synthetic apatites (which are structurally different from bone mineral) and non-physiological conditions have led to contradictory results. Here, we report on the formation of a new Sr 2+-rich and stable amorphous calcium phosphate phase, Sr(ACP). Relying on a bioinspired pathway, a series of Sr 2+ substituted hydroxya-patite (HA) that combines the major bone mineral features is depicted as model to investigate how this phase forms and Sr 2+ affects bone. In addition, by means of a comprehensive investigation the biominer-alization pathway of Sr 2+ bearing HA is described showing that not more than 10 at% of Sr 2+ , i.e. a physiological limit incorporated in bone, can be incorporated into HA without phase segregation. A combination of 31 P and 1 H solid state NMR, energy electron loss spectromicroscopy, transmission electron microscopy, electron diffraction, and Raman spectroscopy shows that Sr 2+ introduces disorder in the HA culminating with the unexpected Sr(ACP), which co-exists with the HA under physiological conditions. These results suggest that heterogeneous Sr 2+ distribution in bone is associated with regions of low structural organization. Going further, such observations give clues from the physicochemical standpoint to understand the defects in bone formation induced by high Sr 2+ doses. Statement of Significance Understanding the role played by Sr 2+ has a relevant impact in physiological biomineralization and provides insights for its use as osteoporosis treatments. Previous studies inspired by the bone remodelling pathway led to the formation of biomimetic HA in terms of composition, structures and properties in water. Herein, by investigating different atomic percentage of Sr 2+ related to Ca 2+ in the synthesis, we demonstrate that 10% of Sr 2+ is the critical loads into the biomimetic HA phase; similarly to bone. Unexpectedly, using higher amount leads to the formation of a stable Sr 2+-rich amorphous calcium phosphate phase that may high-dose related pathologies. Our results provide further understanding of the different ways Sr 2+ impacts bone.
Published: 2019

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