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84 results on '"Electrochimie Interfaciale et Procédés (EIP )"'

1. Utilization of Torrefied Coffee Grounds as Reinforcing Agent To Produce High-Quality Biodegradable PBAT Composites for Food Packaging Applications

Author

Chamseddine Guizani, Alain Dufresne, Hesham Moustafa, Vincent Martin, Mejdi Jeguirim, Capucine Dupont, Laboratoire Génie des procédés papetiers (LGP2), Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), CEA- Saclay (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institut de Science des Matériaux de Mulhouse (IS2M), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-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), ANR-11-CARN-030-01 - Matériaux bio-sourcés fonctionnels - PolyNat Carnot Institute, ANR-11-LABX-0030,TEC XXI,Ingénierie de la Complexité : la mécanique et ses interfaces au service des enjeux sociétaux du 21iè(2011), 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, Laboratoire Génie des procédés papetiers (LGP2 ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS), Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), 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, and 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)

Subjects
Materials science, Scanning electron microscope, General Chemical Engineering, Melting temperature, Hydrophobicity, Mechanical properties, 02 engineering and technology, Torrefaction coffee grounds, 010402 general chemistry, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, Contact angle, Crystallinity, Coffee grounds, Differential scanning calorimetry, [CHIM]Chemical Sciences, Environmental Chemistry, PBAT, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, Composite material, TGA, Renewable Energy, Sustainability and the Environment, Thermo-mechanical properties, General Chemistry, 021001 nanoscience & nanotechnology, Torrefaction, 0104 chemical sciences, Food packaging, 0210 nano-technology
Abstract

International audience; The present study has revealed that torrefied coffee grounds (CG) derived from agriculture commodities can be used as bioreinforcing agent for biodegradable poly(butylene adipate-co-terephthalate) (PBAT) without requiring a compatibilizer. The optimum torrefaction operation was achieved in order to increase the hydrophobicity of CG. The raw CG was also used as a reference to assess the effect of the torrefaction operation. The structure and morphology of the composites were examined by X-ray diffraction (XRD) and scanning electron microscopy (SEM), respectively. The effect of the addition of raw or torrefied CG on the melting temperature and crystallinity of PBAT biocomposites was analyzed by differential scanning calorimetry (DSC). A significant enhancement in the thermo-mechanical properties for PBAT/torrefied CG composites was observed compared to PBAT/CG composites. Moreover, the hydrophobicity of PBAT composites which was determined by water contact angle was improved when torrefied biomass was added. The thermal stability of the investigated samples was analyzed by thermogravimetric analysis (TGA) and a kinetic model was proposed to describe the thermal degradation of raw CG, torrefied CG, PBAT, and their filled composites. The obtained results for these solvent-free prepared biocomposites show that they can be potential candidates for food packaging applications.

Published
2017
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2. Electrochemical Strain Dynamics in Noble Metal Nanocatalysts

Author

Guillaume Braesch, H. Isern, Isaac Martens, Florian Russello, Jakub Drnec, Michal Ronovsky, Veijo Honkimäki, Marta Mirolo, Eric Sibert, Elisabeth Hornberger, Marian Chatenet, Raphaël Chattot, Peter Strasser, European Synchroton Radiation Facility [Grenoble] (ESRF), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Technische Universität Berlin (TU)

Subjects
Chemistry, Nanotechnology, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Chemistry, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 7. Clean energy, Biochemistry, Catalysis, Nanomaterial-based catalyst, 0104 chemical sciences, Colloid and Surface Chemistry, Adsorption, engineering, Energy transformation, Noble metal, Cyclic voltammetry, 0210 nano-technology, Absorption (electromagnetic radiation), ComputingMilieux_MISCELLANEOUS
Abstract

The theoretical design of effective metal electrocatalysts for energy conversion and storage devices relies greatly on supposed unilateral effects of catalysts structure on electrocatalyzed reactions. Here, by using high-energy X-ray diffraction from the new Extremely Brilliant Source of the European Synchrotron Radiation Facility (ESRF-EBS) on device-relevant Pd and Pt nanocatalysts during cyclic voltammetry experiments in liquid electrolytes, we reveal the near ubiquitous feedback from various electrochemical processes on nanocatalyst strain. Beyond challenging and extending the current understanding of practical nanocatalysts behavior in electrochemical environment, the reported electrochemical strain provides experimental access to nanocatalysts absorption and adsorption trends (i.e., reactivity and stability descriptors) operando. The ease and power in monitoring such key catalyst properties at new and future beamlines is foreseen to provide a discovery platform toward the study of nanocatalysts encompassing a large variety of applications, from model environments to the device level.

Published
2021
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3. Impact of ionomer structuration on the performance of bio-inspired noble-metal-free fuel cell anodes

Author

Vincent Artero, Fabrice Valentino, Tristan Asset, Tran Ngoc Huan, Nathan Coutard, Bruno Jousselme, Sandrine Lyonnard, Bertrand Reuillard, Pascale Chenevier, Reuben T. Jane, Eugen S. Andreiadis, Solène Gentil, Alan Le Goff, Adina Morozan, Frédéric Maillard, Solar fuels, hydrogen and catalysis (SolHyCat), Laboratoire de Chimie et Biologie des Métaux (LCBM - UMR 5249), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Département de Chimie Moléculaire (DCM), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), ANR-17-EURE-0003,CBH-EUR-GS,CBH-EUR-GS(2017), European Project, Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)

Subjects
Materials science, Nanotechnology, 02 engineering and technology, Carbon nanotube, engineering.material, 010402 general chemistry, 7. Clean energy, 01 natural sciences, law.invention, Catalysis, chemistry.chemical_compound, law, Nafion, Ionomer, General Environmental Science, Nanocomposite, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, Chronoamperometry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Anode, chemistry, engineering, General Earth and Planetary Sciences, Noble metal, 0210 nano-technology
Abstract

https://www.sciencedirect.com/science/article/pii/S2667109321000014?via%3Dihub; International audience; Molecular-engineered bio-inspired catalysts hold promise for the next generation of proton-exchange membrane fuel cells (PEMFCs). Yet, their implementation in catalytic layers with Nafion ionomer faces nanocomposite formulation issues. Here, we use various DuBois nickel catalysts immobilized on carbon nanotubes to exemplify how self-assembly at the mesoscale affects H2 oxidation anode performance. We exploited the reversible activity of these catalysts together with potential-step chronoamperometry to locally produce H2 and probe mass transport within the catalyticlayer. Small-angle neutron scattering studies serve to build a model describing how the surface functionalization drives the structuration of the ionomer and affects the diffusion of protons and gas from and to catalytic centers. This study thus demonstrates that implementation of unconventional catalysts in catalytic layers requires the redesign of the whole system of materials. On the basis of such information, catalytic layer formulation was optimized,allowing order-of-magnitude performance enhancement of noble-metal-free PEMFCs

Published
2021
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4. Use of magnetic fields in electrochemistry: A selected review

Author

Vivien Gatard, Jonathan Deseure, Marian Chatenet, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Convection, Materials science, Kinetics, Electrochemical kinetics, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrocatalyst, Electrochemistry, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Analytical Chemistry, Forced convection, Magnetic field, Chemical physics, [CHIM]Chemical Sciences, Physics::Chemical Physics, 0210 nano-technology, Spin (physics), ComputingMilieux_MISCELLANEOUS
Abstract

Electrochemical reactions are usually thermally activated and submitted to mass-transfer effects. Although classically, enhanced kinetics of an electrochemical reaction is obtained by heating the cell and feeding the reactant by forced convection, other means can be used to improve mass-transfer and charge-transfer. This article shortly reviews the effects of magnetic fields in electrochemistry. Using a static or an alternating magnetic field enables to enhance electrodeposition and electrocatalysis, via improved gas and species convection, electrochemical kinetics, and whole reaction efficiency. Such enhancement can mainly be related to Lorentz and Kelvin forces, magneto-hydrodynamics, chiral-induced spin selectivity, and hyperthermia, these effects being described herein.

Published
2020
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5. Selective Separation of Manganese, Cobalt, and Nickel in a Fully Aqueous System

Author

Lenka Svecova, Matthieu Gras, João A. P. Coutinho, Márcia C. Neves, Silvia J. R. Vargas, Helena Passos, Nicolas Papaiconomou, Nicolas Schaeffer, Centre for Nanoscale Science, University of Liverpool, Universidade de Aveiro, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Laboratoire de Chimie Moléculaire et Environnement (LCME), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), and CICECO

Subjects
Aqueous solution, Materials science, 010405 organic chemistry, Renewable Energy, Sustainability and the Environment, Battery recycling, General Chemical Engineering, chemistry.chemical_element, Aqueous biphasic system, Cobalt, General Chemistry, Manganese, 010402 general chemistry, 01 natural sciences, Metal separation, 0104 chemical sciences, 12. Responsible consumption, Nickel, chemistry, Chemical engineering, Selective precipitation, [CHIM]Chemical Sciences, Environmental Chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

The continued electrification of society and the related growing demand for rechargeable batteries require in turn the elaboration of efficient and sustainable recycling strategies for their recovery and valorization. An important separation relevant to nickel metal hydride (NiMH) and lithium-ion battery recycling is the intertransition element separation between Ni(II), Co(II), and Mn(II). In this work, a fully aqueous process for the recovery of Mn(II) and Co(II) from concentrated Ni(II) effluents typical of NiMH battery leachate is disclosed consuming only Na2CO3. In the first instance, Mn is selectively precipitated as Mn(IV) by oxidation using ozone as an oxidant, resulting in a significant enrichment of Mn in the precipitate relative to its original solution concentration. Second, a thermo- and acid-responsive aqueous biphasic system (ABS) based on the ionic liquid (IL) tributyltetradecylphosphonium chloride ([P44414]Cl) and NiCl2 was used to recover Co(II). By using the high NiCl2 content found in NiMH leachates both as the ABS phase former and salting-out agent, no additional salt is required. Through careful manipulation of the Co(II) to Ni(II) and the IL to Co(II) molar ratios, an effective and selective separation of Co(II) from Ni(II) was achieved. Finally, Co(II) is precipitated from the IL-rich phase and the IL is regenerated in one step by the addition of Na2CO3 to induce a new phase separation. published

Published
2020
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6. Simplified anode architecture for PEMFC systems based on alternative fuel feeding: Experimental characterization and optimization for automotive applications

Author

Y. Bultel, Jean-Philippe Poirot-Crouvezier, S. Rodosik, Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)

Subjects
Test bench, Computer science, Automotive industry, Energy Engineering and Power Technology, Proton exchange membrane fuel cell, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Automotive engineering, law.invention, [SPI]Engineering Sciences [physics], Stack (abstract data type), law, Sensitivity (control systems), ComputingMilieux_MISCELLANEOUS, Renewable Energy, Sustainability and the Environment, business.industry, Injector, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Durability, 0104 chemical sciences, Anode, Fuel Technology, 0210 nano-technology, business
Abstract

The need to reduce PEMFC systems cost as well as to increase their durability is crucial for their integration in various applications and especially for transport applications. A new simplified architecture of the anode circuit called Alternating Fuel Feeding (AFF) offers to reduce the development costs. Requiring a new stack concept, it combines the simplicity of Dead-End Anode (DEA) with the operation advantages of the hydrogen recirculation. The three architectures (DEA, recirculation and AFF) are compared in terms of performance on a 5-kW test bench in automotive conditions, through a sensitivity analysis. A gain of 17% on the system efficiency is observed when switching from DEA to AFF. Moreover, similar performances are obtained both for AFF and for recirculation after an accurate optimization of the AFF tuning parameters. Based on DoE data, a gain of 25% on the weight of the anodic line has been identified compared to pulsed ejector architecture and 43% with the classic recirculation architecture with blower only (Mirai).

Published
2020
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7. Recent Advances in the Understanding of Nickel-Based Catalysts for the Oxidation of Hydrogen-Containing Fuels in Alkaline Media

Author

Marian Chatenet, Elena R. Savinova, Antoine Bonnefont, Guillaume Braesch, Alexandr G. Oshchepkov, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Materials science, Hydrogen, chemistry.chemical_element, Nickel based, 010402 general chemistry, Electrochemistry, 7. Clean energy, 01 natural sciences, Catalysis, Physics::Geophysics, Metal, Condensed Matter::Materials Science, Transition metal, Physics::Chemical Physics, ComputingMilieux_MISCELLANEOUS, 010405 organic chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, 0104 chemical sciences, Nickel, chemistry, Chemical engineering, visual_art, visual_art.visual_art_medium, Condensed Matter::Strongly Correlated Electrons, Astrophysics::Earth and Planetary Astrophysics, Earth (classical element)
Abstract

Nickel is a very abundant transition metal in the Earth’s crust, and it finds numerous applications in electrochemical processes where metallic Ni or its oxides are thermodynamically stable, partic...

Published
2020
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8. On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts

Author

Jingkun Li, Kavita Kumar, Michel Mermoux, Frédéric Jaouen, Jaysen Nelayah, Frédéric Maillard, Andrea Zitolo, Laetitia Dubau, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Matériaux Interfaces ELectrochimie (MIEL), 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), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Matériaux et Phénomènes Quantiques (MPQ (UMR_7162)), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Projet ANR CAT2CAT (ANR-16-CE05-0007)Projet ANR ANIMA (ANR-19-CE05-0039), ANR-16-CE05-0007,CAT2CAT,Des catalyseurs aux cathodes: Une approche d'architecture contrôlée d'électrode pour pile PEM à base de métaux abondants(2016), ANR-19-CE05-0039,ANIMA,Aérogels de carbone poreux dopés à l'azote et avec des métaux abondants pour des assemblages membrane-électrodes efficaces et durables(2019), Université Grenoble Alpes (UGA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut National Polytechnique de Grenoble (INPG)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Centre National de la Recherche Scientifique (CNRS), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), and ANR-19-CE05-0039,ANIMA,ANR-19-CE05-0039 - ANIMA - Aérogels de carbone poreux dopés à l'azote et avec des métaux abondants pour des assemblages membrane-électrodes efficaces et durables

Subjects
Inorganic chemistry, Proton exchange membrane fuel cell, chemistry.chemical_element, Electrolyte, 02 engineering and technology, 010402 general chemistry, Oxygen, 7. Clean energy, 01 natural sciences, Catalysis, Corrosion, symbols.namesake, 010405 organic chemistry, General Medicine, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, 13. Climate action, symbols, Reversible hydrogen electrode, Degradation (geology), Raman spectroscopy, 0210 nano-technology
Abstract

International audience; Precious metal-free catalysts for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells are gaining momentum, with Fe-N-C catalysts comprising atomic FeN x sites the most promising candidate. Research and development is shifting from activity targets to improved stability of Fe-N-C catalysts in fuel cells. Their durability has hitherto been extensively studied using accelerated stress tests (AST) performed at room temperature and in inert-gas saturated acidic pH electrolyte. Here, we reveal stronger degradation of the Fe-N-C structure and four times higher ORR activity loss when performing load cycling AST in O2-vs. Ar-saturated pH 1 electrolyte. Raman spectroscopy results point towards strong carbon corrosion after AST in O2 , even when cycling at low potentials of 0.3-0.7 V vs. the reversible hydrogen electrode, while no corrosion occurred after any load cycling AST in Ar. The load cycling AST in O2 leads to the loss of a significant fraction of FeN x sites, as shown by energy dispersive X-ray spectroscopy analyses, and to the formation of Fe oxides. The results support that the unexpected carbon corrosion occurring at such low potential in the presence of O2 is due to reactive oxygen species produced between H 2 O 2 and Fe sites via Fenton reactions.

Published
2020
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9. Tailoring the Oxygen Reduction Activity of Pt Nanoparticles through Surface Defects: A Simple Top-Down Approach

Author

Regina M. Kluge, Weijin Li, Jan Michalička, Hany A. El-Sayed, Raphaël Chattot, Thomas Gigl, Aliaksandr S. Bandarenka, Felix Haimerl, Batyr Garlyyev, Di Wang, Christoph Hugenschmidt, Wu Wang, Jan M. Macak, Johannes Fichtner, Sebastian Watzele, Laetitia Dubau, Frédéric Maillard, Technische Universität Munchen - Université Technique de Munich [Munich, Allemagne] (TUM), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), European Synchrotron Radiation Facility (ESRF), Central European Institute of Technology [Brno] (CEITEC MU), Brno University of Technology [Brno] (BUT), Institute of Nanotechnology [Karlsruhe] (INT), Karlsruhe Institute of Technology (KIT), and Forschungszentrum Julich, Heinz Maier Leibnitz Zentrum MLZ, JCNS, Lichtenbergstr 1, D-85747 Garching, Germany

Subjects
Surface (mathematics), Technology, Materials science, 010405 organic chemistry, Kinetics, food and beverages, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, 2019-022-025989, 010402 general chemistry, Platinum nanoparticles, Electrocatalyst, 01 natural sciences, Catalysis, Oxygen reduction, 0104 chemical sciences, Chemical engineering, TEM, Oxygen reduction reaction, Pt nanoparticles, ddc:600, ComputingMilieux_MISCELLANEOUS
Abstract

Results from Pt model catalyst surfaces have demonstrated that surface defects, in particular surface concavities, can improve the oxygen reduction reaction (ORR) kinetics. It is, however, a challe...

Published
2020
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10. Direct borohydride fuel cells: A selected review of their reaction mechanisms, electrocatalysts, and influence of operating parameters on their performance

Author

Antoine Bonnefont, Elena R. Savinova, Marian Chatenet, Alexandr G. Oshchepkov, Gaël Maranzana, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Reaction mechanism, Materials science, 02 engineering and technology, 010402 general chemistry, Borohydride, Electrocatalyst, 01 natural sciences, 7. Clean energy, Redox, Analytical Chemistry, Catalysis, Sodium borohydride, chemistry.chemical_compound, Nickel, Electrochemistry, Direct Borohydride Fuel Cells, Platinum, Hydrogen escape, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Anode, Membrane, Chemical engineering, chemistry, Borohydride Oxidation Reaction, 0210 nano-technology, Palladium
Abstract

International audience; Direct borohydride fuel cells (DBFC) oxidize an easily-stored energy-dense borohydride fuel (sodium borohydride: NaBH4), that in theory reacts ca. 400 mV below H2 and produce 8 electrons per BH4anion. However, the borohydride oxidation reaction (BOR) does not fully meet these promises in practice: the electrocatalyst nature, structure and state-of-surface, and the operating conditions (pH, BH4concentration, temperature, fluxes) noticeably influence the BOR kinetics and mechanism. Nickel and platinum-based catalysts both have assets for the BOR. DBFCs can only yield decent performance if their separator combines high ionconductivity and efficient separation of the reactants; cation-exchange membranes, anionexchange membranes, bipolar membranes and porous separators all have their own advantages and drawbacks. Besides the anode, the choice of separator must consider the DBFC cathode reaction, where oxygen (air) or hydrogen peroxide are reduced, provided adapted catalysts are used. All these aspects drive the DBFC performance and stability/durability.

Published
2022
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11. Bimetallic Pt or Pd-based carbon supported nanoparticles are more stable than their monometallic counterparts for application in membraneless alkaline fuel cell anodes

Author

Ronit Sharabi, Marian Chatenet, Huong Doan, Yair Haim Wijsboom, Nino Borchtchoukova, Thiago Morais, Gennadi Finkelshtain, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Universidade de São Paulo (USP)

Subjects
Alkaline fuel cell, Nanoparticle, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Catalysis, Durability, Metal, Hydrogen oxidation reaction, Bimetallic strip, Dissolution, General Environmental Science, Chemistry, Process Chemistry and Technology, Poisoning, Platinum group metal catalysts, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, visual_art, visual_art.visual_art_medium, 0210 nano-technology, Carbon
Abstract

International audience; Alkaline fuel cells (AFCs) are relevant for niche applications, but still require enhanced performance and lifetime. Active and durable hydrogen oxidation reaction (HOR) catalysts must be developed: linking their electrochemical surface area (ECSA) loss to their HOR activity and understanding whether the ECSA loss of carbonsupported platinum group metal-based (PGM/C) HOR catalysts is irreversible (nanoparticles dissolution, detachment, Ostwald ripening) or reversible is pivotal. Using identical-location transmission electron micrographs (IL-TEM) and ECSA characterizations by "CO-like" stripping undertaken pre and post accelerated stress tests (AST), the different degradation mechanisms undergone by monometallic (Pt/C and Pd/C) and bimetallic catalysts (Pd-Pt/C and Pd-Ni/C) are unveiled. Monometallic PGM/C undergo extensive reversible poisoning and irreversible degradation upon operation at low potential, in contrast to bimetallic catalysts, which are less affected. Pd-Ni exhibits the smallest loss of ECSA PGM and HOR activity: it poorly catalyzes carbon corrosion and is hardly poisoned by "CO-like" species.

Published
2022
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12. FeNi3 and Ni-based nanoparticles as electrocatalysts for magnetically-enhanced alkaline water electrolysis

Author

Vivien Gatard, Déborah De Masi, Raphaël Chattot, Irene Mustieles Marin, Juan Manuel Asensio Revert, Pier-Francesco Fazzini, Thierry Encinas, Vincent Martin, Stéphane Faure, Jonathan Deseure, Julian Carrey, Bruno Chaudret, Marian Chatenet, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Laboratoire de physique et chimie des nano-objets (LPCNO), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), and Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)

Subjects
Materials science, Electrolysis of water, Hydrogen, Alkaline water electrolysis, Oxygen evolution, chemistry.chemical_element, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Catalysis, chemistry, Chemical engineering, 13. Climate action, Rotating disk electrode, Inductively coupled plasma, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

Today, hydrogen mainly originates from fossil sources (gas, oil, and coal). Room temperature water electrolysis is an interesting alternative for renewable electricity storage, even if it is well-known that high-temperature systems are more efficient. To address this issue, we studied different non-platinum group metal (non-PGM) catalysts for alkaline oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) by recording cyclic voltamperograms with a rotating disk electrode set up. Physicochemical characterizations of Ni-based and FeNi3-based catalysts were performed using transmission electron microscopy, X-ray diffraction (XRD), and inductively coupled plasma mass spectroscopy (ICP-MS). Ni synthesized by the hot injection method is a good catalyst for HER, yet still less active than Pt/C. FeNi3 with and without a Ni surface doping is very good OER catalysts, slightly better than commercial unsupported IrO2. Electrochemical tests under alternating magnetic field (AMF) using these nanoparticles are ongoing, as these materials are compatible with AMF activation.

Published
2021
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13. Insights into the borohydride electrooxidation reaction on metallic nickel from operando FTIRS, on-line DEMS and DFT

Author

Gholamreza Rostamikia, Elena R. Savinova, Marian Chatenet, Antoine Bonnefont, Alexandr G. Oshchepkov, Michael J. Janik, Guillaume Braesch, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Centre National de la Recherche Scientifique (CNRS)-Université Louis Pasteur - Strasbourg I-Institut de Chimie du CNRS (INC), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-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)-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), Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences (SB RAS), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Pennsylvania State University (Penn State), and Penn State System

Subjects
Materials science, General Chemical Engineering, Inorganic chemistry, Infrared spectroscopy, 02 engineering and technology, 010402 general chemistry, Borohydride, Electrochemistry, Mass spectrometry, 7. Clean energy, 01 natural sciences, Redox, Metal, chemistry.chemical_compound, Density Functional Theory calculations, Borohydride oxidation reaction, polycrystalline nickel electrode, ComputingMilieux_MISCELLANEOUS, Line (formation), Fourier Transform Infrared Spectroscopy, Differential Electrochemical Mass Spectrometry, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, visual_art, visual_art.visual_art_medium, Density functional theory, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other
Abstract

International audience; Direct Borohydride Fuel Cells (DBFCs) are considered as promising power sources for portable and mobile applications. Their advantages are high theoretical energy density, and high theoretical cell voltage. Metallic Ni has recently emerged as a promising electrode material for DBFCs. In this work we combine electrochemical, operando Fourier-Transform infrared spectroscopy (FTIRS), and online differential electrochemical mass spectrometry (DEMS) measurements with density functional theory (DFT) calculations to advance the understanding of the borohydride oxidation reaction on Ni.

Published
2021
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14. Thin Tantalum Film Electrodeposition from an Ionic Liquid—Influence of Substrate Nature, Electrolyte Temperature and Electrochemical Parameters on Deposits’ Quality

Author

Lenka Svecova, Maguy Nahra, Eric Chainet, Nicolas Sergent, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Matériaux Interfaces ELectrochimie (MIEL)

Subjects
Materials science, Tantalum, chemistry.chemical_element, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, law.invention, chemistry.chemical_compound, symbols.namesake, X-ray photoelectron spectroscopy, law, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Materials Chemistry, Electrolysis, Renewable Energy, Sustainability and the Environment, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Tantalum pentafluoride, chemistry, Chemical engineering, Ionic liquid, symbols, 0210 nano-technology, Raman spectroscopy
Abstract

International audience; This paper discusses the feasibility of tantalum electrodeposition carried out under potential control from 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide [BMPyr][TFSI] room temperature ionic liquid electrolyte containing tantalum pentafluoride (TaF5). The influence of electrode nature, electrolyte temperature and electrolysis duration on the morphology, the adherence, the thickness and the crystalline properties of tantalum deposits is reported. The obtained tantalum deposits are analyzed by SEM, XRD, Raman spectroscopy and XPS surface analytical techniques. Pulsed potential electrodeposition is investigated in order to enhance deposit properties. Post electrodeposition thermal treatments are also reported.

Published
2021
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15. Durability challenges of anion exchange membrane fuel cells

Author

William E. Mustain, Yu Seung Kim, Marian Chatenet, Miles Page, University of South Carolina [Columbia], Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Los Alamos National Laboratory (LANL)

Subjects
Ion exchange, Renewable Energy, Sustainability and the Environment, business.industry, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Proton exchange membrane fuel cell, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, Limiting, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, Pollution, Durability, 0104 chemical sciences, Membrane, Nuclear Energy and Engineering, Environmental Chemistry, Environmental science, Fuel cells, 0210 nano-technology, Process engineering, business
Abstract

International audience; As substantial progress has been made in improving the performance of anion exchange membrane fuel cells (AEMFCs) over the last decade, the durability of AEMFCs has become the most critical requirement to deploy competitive energy conversion systems. Because of different operating environments from proton exchange membrane fuel cells, several AEMFC-specific component degradations have been identified as the limiting factors influencing the AEMFC durability. In this article, AEMFC durability protocol, the current status of AEMFC durability, and performance degradation mechanisms are reported based on the discussion during the US Department of Energy (DOE) Anion Exchange Membrane Workshop at Dallas, Texas, May 2019. With additional recent progress, we provide our perspectives on current technical challenges and future action to develop long-lasting AEMFCs.

Published
2020
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16. Disclosing Pt-Bimetallic Alloy Nanoparticle Surface Lattice Distortion with Electrochemical Probes

Author

Frédéric Maillard, Isaac Martens, Juan Herranz, Raphaël Chattot, Marion Scohy, Jakub Drnec, Laetitia Dubau, European Synchrotron Radiation Facility (ESRF), Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), and Institut National de la Recherche Scientifique [Québec] (INRS)

Subjects
Imagination, Chemical substance, Materials science, Renewable Energy, Sustainability and the Environment, media_common.quotation_subject, Alloy nanoparticle, Lattice distortion, Energy Engineering and Power Technology, Nanotechnology, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 0104 chemical sciences, Catalysis, Fuel Technology, Chemistry (miscellaneous), Materials Chemistry, 0210 nano-technology, Science, technology and society, Bimetallic strip, media_common
Abstract

International audience; Structural defects are of significant importance in(electro)catalysis, as they provide sites of unusually high activity thatfind applications in many key electrochemical processes. However,tools to characterize surface defects remain scarce and complex,especially for nanocatalysts where classical methods such astransmission electron microscopy or X-ray scattering are limited intheir ability to probe the structure and distribution of the activesurface sites. Herein, we show that the ratio between the COadsstripping charge (QCO) and the charge required to desorb underpotentiallydeposited H atoms (QH) in structurally disordered Ptbasednanocatalysts scales almost linearly with the surface distortiondescriptor obtained via advanced physical methods. This trend isvalid in both rotating disk electrode configuration and in a real fuelcell device, thus providing the scientific community with a powerfuland versatile approach for semiquantitative estimation of the surface lattice distortion in Pt-based catalysts without theneed for exhaustive structural characterization.

Published
2019
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17. Oxygen reduction reaction mechanism and kinetics on M-NxCy and M@N-C active sites present in model M-N-C catalysts under alkaline and acidic conditions

Author

Edson A. Ticianelli, Andrea Zitolo, Frédéric Maillard, Kavita Kumar, Ricardo Sgarbi, Frédéric Jaouen, Instituto de Química de São Carlos, Universidade de São Paulo, Avenida Trabalhador São-Carlense 400, São Carlos, SP, Brazil, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), 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), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), ANR-16-CE05-0007,CAT2CAT,Des catalyseurs aux cathodes: Une approche d'architecture contrôlée d'électrode pour pile PEM à base de métaux abondants(2016), and ANR-19-CE05-0039,ANIMA,Aérogels de carbone poreux dopés à l'azote et avec des métaux abondants pour des assemblages membrane-électrodes efficaces et durables(2019)

Subjects
Kinetics, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, Reaction intermediate, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Catalysis, Metal, Oxygen reduction reaction, General Materials Science, Electrical and Electronic Engineering, COMBUSTÍVEIS, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, chemistry, visual_art, Electrode, visual_art.visual_art_medium, 0210 nano-technology, Carbon
Abstract

International audience; M-N-C electrocatalysts (where M is Fe or Co) have been investigated for mitigating the dependence on noble metals when catalyzing the oxygen reduction reaction (ORR) for fuel cell technologies in acidic or alkaline conditions. Rotating disc and rotating ring-disk electrodes measurements for Fe-N-C and CoN -C catalysts demonstrate promising performances and stability for the ORR, while the activity of main suspected active sites (M-NxCy and M@N-C) has been discussed on the basis of the known physical-chemical properties of the catalysts in acid and alkaline media. Thereupon, it is observed that atomically-dispersed Fe-NxCy sites reach the highest ORR activity in acid media when amplified by an adequate energy binding between the metallic center and the oxygenated reaction intermediates. In contrast, Fe@N-C core-shell sites reach a maximum ORR mass activity in alkaline media through a synergistic effect involving catalyst particles with metallic iron in the core and nitrogen-doped carbon in the shell.

Published
2019
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18. Probing Surface Oxide Formation and Dissolution on/of Ir Single Crystals via X-ray Photoelectron Spectroscopy and Inductively Coupled Plasma Mass Spectrometry

Author

Bruno Gilles, Laetitia Dubau, Sofyane Abbou, Vincent Martin, Marion Scohy, Frédéric Maillard, Eric Sibert, Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Science et Ingénierie des Matériaux et Procédés (SIMaP ), and Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])

Subjects
Materials science, 010405 organic chemistry, Analytical chemistry, Oxygen evolution, chemistry.chemical_element, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, 010402 general chemistry, Electrocatalyst, 01 natural sciences, Catalysis, 0104 chemical sciences, X-ray photoelectron spectroscopy, chemistry, Iridium, Single crystal, Inductively coupled plasma mass spectrometry, Dissolution, ComputingMilieux_MISCELLANEOUS
Abstract

Gaining fundamental insights into the formation and the stability of surface oxides on iridium (Ir) surfaces is pivotal to oxygen evolution reaction (OER) electrocatalysis. Herein, we examined the ...

Published
2019
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19. Surface anodization of the biphasic Ti13Nb13Zr biocompatible alloy: Influence of phases on the formation of TiO2 nanostructures

Author

Virginie Roche, Diego Alfonso Godoy Pérez, Jean-Claude Leprêtre, Claudemiro Bolfarini, Alberto Moreira Jorge Junior, Gabriel Hitoshi Asato, Walter Jose Botta, Universidade Federal de São Carlos [São Carlos] (UFSCar), Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), and Matériaux Interfaces ELectrochimie (MIEL )

Subjects
Anatase, Materials science, Anodizing, Mechanical Engineering, Alloy, Metals and Alloys, 02 engineering and technology, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, Microstructure, 01 natural sciences, 0104 chemical sciences, Amorphous solid, Corrosion, Chemical engineering, Mechanics of Materials, Rutile, Materials Chemistry, Pitting corrosion, engineering, [CHIM]Chemical Sciences, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

Here we report for the first time that the anodization of the biphasic (α'+β) Ti13Nb13Zr alloy form arrays of TiO2 nanotubes with well-defined circular geometry in the α′ phase, while nanopores of TiO2 are formed in the β phase. Samples of the Ti13Nb13Zr alloy were severely plastic deformed using High-Pressure Torsion (HPT) to refine the microstructure and to redistribute α′ and β phases. The anodization was performed using an organic electrolyte (glycerol) containing fluoride ions and a few percentages of water. All the specimens coated with nanotubes were annealed at 550 °C to crystallize the modified surface of the as-anodized samples. XRD analyses confirmed that the as-anodized amorphous nanostructures crystallize in a mixture of anatase and rutile after heat treatment, and SEM observations showed no significant morphological changes in the surface phases. The evaluation of corrosion resistance showed that anodized samples have much better corrosion properties than polished ones without any evidence of pitting corrosion. Quantitative comparison between anodized coarse-grained (α'+β)-Ti alloy and ultra-fine grained (α'+β)-Ti one showed that the nanostructuring of the (α'+β)-Ti alloy by HPT helped to improve the bioactivity when compared with the coarse-grained sample.

Published
2019
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20. Nickel Metal Nanoparticles as Anode Electrocatalysts for Highly Efficient Direct Borohydride Fuel Cells

Author

Gholamreza Rostamikia, Vasiliki Papaefthimiou, Alexandr G. Oshchepkov, Marian Chatenet, Michael J. Janik, Gaël Maranzana, Guillaume Braesch, Elena R. Savinova, Salem Ould-Amara, Antoine Bonnefont, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), 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), Pennsylvania State University (Penn State), Penn State System, Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), and Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, 010405 organic chemistry, chemistry.chemical_element, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, 010402 general chemistry, Borohydride, 7. Clean energy, 01 natural sciences, Redox, Catalysis, 0104 chemical sciences, Anode, chemistry.chemical_compound, Nickel, chemistry, Chemical engineering, Direct borohydride fuel cell, Platinum, ComputingMilieux_MISCELLANEOUS, Palladium
Abstract

Developing cost-effective electrocatalysts for the multielectron borohydride oxidation reaction (BOR) is mandatory to deploy direct borohydride fuel cell (DBFC) systems to power portable and mobile...

Published
2019
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21. Degradation of Carbon-Supported Platinum-Group-Metal Electrocatalysts in Alkaline Media Studied by in Situ Fourier Transform Infrared Spectroscopy and Identical-Location Transmission Electron Microscopy

Author

Vincent Martin, Clémence Lafforgue, Laetitia Dubau, Frédéric Maillard, Marian Chatenet, Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), and Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])

Subjects
In situ, Materials science, chemistry.chemical_element, alkaline fuel cells, 010402 general chemistry, Electrochemistry, 01 natural sciences, Catalysis, Metal, Fourier transform infrared spectroscopy, identical-location transmission electron microscopy, 010405 organic chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, degradation mechanism, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry, Chemical engineering, Transmission electron microscopy, visual_art, visual_art.visual_art_medium, Degradation (geology), PGM-containing carbon-supported electrocatalyst, Carbon
Abstract

International audience; Alkaline fuel cells and electrolyzers have attracted increasing attention from the electrochemical community, and one of their supposed advantages is their greater electrode material stability in comparison to their proton-exchange membrane analogues. However, the stability of the core materials of fuel cells and electrolyzers in an alkaline environment cannot be taken for granted and remains understudied so far. Herein, using in situ Fourier transform infrared spectroscopy (FTIR), identical-location transmission electron microscopy (IL-TEM), X-ray photoelectron spectroscopy (XPS), and COads stripping techniques, we provide physical and chemical evidence that Pt-based nanocatalysts catalyze the electrochemical corrosion of the carbon support (Vulcan XC72). This is due to more facile oxidation of oxygen-containing surface groups of the carbon support upon adsorption of hydroxyl groups on the Pt-based surface. The degradation mechanism is, to some extent, similar for other carbon-supported Pt-group metal (PGM) electrocatalysts. We propose that the extent of degradation of PGM/C nanoparticles in alkaline electrolytes scales with the electrocatalyst’s activity to electrooxidize CO, thereby providing a marker of the material’s propensity for degradation in an alkaline environment.

Published
2019
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22. Study of sulfur-based electrodes by operando acoustic emission

Author

Fannie Alloin, Pierre-Xavier Thivel, Hassane Idrissi, Lionel Roué, Quentin Lemarié, Institut National de la Recherche Scientifique [Québec] (INRS), Matériaux, ingénierie et science [Villeurbanne] (MATEIS), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-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 Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Matériaux Interfaces ELectrochimie (MIEL ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Electrochimie Interfaciale et Procédés (EIP ), Énergie Matériaux Télécommunications - INRS (EMT-INRS), Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM), Université de Nantes (UN)-Aix Marseille Université (AMU)-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 Montpellier (ENSCM)-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)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)

Subjects
Materials science, Positive electrode formulation, General Chemical Engineering, chemistry.chemical_element, Mechanical properties, Lithium-sulfur batteries, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, Acoustic emission, [CHIM]Chemical Sciences, Composite material, Porosity, Dissolution, ComputingMilieux_MISCELLANEOUS, Current collector, 021001 nanoscience & nanotechnology, Sulfur, 0104 chemical sciences, chemistry, Electrode, 0210 nano-technology
Abstract

The acoustic emission (AE) technique has been widely used since the 70’s for detecting anomalies such as leakages and cracks on large structure (e.g. bridges, pressure containers, and pipe lines). The analysis of the AE signals (transient elastic waves) can also be used to characterize the degradation mechanisms (crack growth, friction, delamination, matrix cracking, corrosion, etc) of various materials subjected to a stress by mechanical, pressure or thermal means. Recently, AE technique has also been used to evaluate the degradation of metal hydride electrodes for Ni-MH [1] and Si-based electrodes for Li-ion batteries [2,3]. Cracking of the active material and gas evolution are the main sources of AE signals identified in these studies. In the present study, the AE technique is used for studying upon cycling the mechanical degradation of S-based electrodes for Li/S batteries. The AE signals were recorded by a piezoelectric transducer fixed on the back of the working electrode. S-based electrodes made with two different binders (PVdF vs. CMC) and two different current collectors (standard Al foil vs. porous 3D carbon paper) were studied. In all cases, AE signals were mainly detected during the first plateau of the first discharge, suggesting that the electrode degradation mostly occurs during the initial dissolution of the S8 particles. AE signals were also detected during a few subsequent cycles when CMC binder is used. This is attributed to a better propagation of the AE signals through the electrode thanks to an improved adhesion of the electrode to the current collector in comparison to PVdF binder. This is confirmed by further mechanical resistance testing (peel and scratch tests). The use of a carbon paper as a current collector combined to CMC binder greatly improves the electrochemical performance of the S electrode by preventing the collapse of the electrode upon cycling. This electrode also presents an increased amount of AE signals, suggesting that the carbon fibres of the C paper act as an AE waveguide. This study demonstrated that AE could be used as an efficient tool to monitor the morphological degradation of S-based electrodes upon their cycling and offers relevant information for optimizing their formulation and architecture. A. Etiemble, H. Idrissi, P. Bernard, L. Roué. New insights into the pulverization of LaNi5-based alloys with different Co contents from electrochemical acoustic emission measurements. Electrochim. Acta 186 (2015) 112-116 A. Tranchot, A. Etiemble, P-X. Thivel, H. Idrissi., L. Roué. In-situ acoustic emission study of Si-based electrodes for Li-ion batteries, J. Power Sources 279 (2015) 259-266. A. Tranchot, P-X. Thivel, H. Idrissi, L. Roué. Influence of the Si particle size on the mechanical stability of Si-based electrodes evaluated by in-operando dilatometry and acoustic emission. J. Power Sources 330 (2016) 253-260. Figure 1

Published
2019
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23. A HNO 3 ‐Responsive Aqueous Biphasic System for Metal Separation: Application towards Ce IV Recovery

Author

Nicolas Schaeffer, Paula Brandão, Silvia J. R. Vargas, João A. P. Coutinho, Papaiconomou, Lenka Svecova, Helena Passos, Helena I. S. Nogueira, Center for Research in Ceramic and Composite Materials (CICECO), Universidade de Aveiro, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institut de Chimie de Nice (ICN), Université Nice Sophia Antipolis (... - 2019) (UNS), and COMUE Université Côte d'Azur (2015-2019) (COMUE UCA)-COMUE Université Côte d'Azur (2015-2019) (COMUE UCA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Côte d'Azur (UCA)

Subjects
General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, Sustainable Chemistry, 01 natural sciences, Metal, Transition metal, Hydrometallurgy, Environmental Chemistry, [CHIM]Chemical Sciences, General Materials Science, ComputingMilieux_MISCELLANEOUS, Aqueous solution, Hydride, Extraction (chemistry), Self-assembly, Electronic waste, 021001 nanoscience & nanotechnology, 6. Clean water, 0104 chemical sciences, Metal separation, Nickel, General Energy, chemistry, visual_art, visual_art.visual_art_medium, Leaching (metallurgy), 0210 nano-technology
Abstract

An acidic aqueous biphasic system (AcABS) presenting a desired and reversible phase transition with HNO3 concentration and temperature was developed herein as an integrated platform for metal separation. The simple, economical, and fully incinerable (C,H,O,N) AcABS composed of tetrabutylammonium nitrate ([N4444][NO3])+HNO3 +H2O was characterized and presented an excellent selectivity towards CeIV against other rare earth elements and transition metals from both synthetic solutions and nickel metal hydride (NiMH) battery leachates. The acid-driven self-assembly of AcABS bridges the gap between traditional ABS and liquid-liquid extraction whilst retaining their advantageous qualities, including compatibility with highly acidic solutions, water as the primary system component, the avoidance of organic diluents, rapid mass transfer, and the potential integration of the leaching and separation steps. published

Published
2021
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24. Imaging Heterogeneous Electrocatalyst Stability and Decoupling Degradation Mechanisms in Operating Hydrogen Fuel Cells

Author

Isaac Martens, Tim Starr, Nicolas Martinez, Janne Pusa, Alan Coelho, Arnaud Morin, Simon D. M. Jacques, Laetitia Dubau, Sandrine Lyonnard, Frédéric Maillard, David P. Wilkinson, Veijo Honkimäki, Dan Bizzotto, Elizabeth A. Fisher, Jakub Drnec, Raphaël Chattot, Sylvie Escribano, Antonis Vamvakeros, Maria Valeria Blanco, Tristan Asset, Fabrice Micoud, European Synchrotron Radiation Facility (ESRF), European Synchroton Radiation Facility [Grenoble] (ESRF), University College of London [London] (UCL), Université Grenoble Alpes (UGA), Institut Laue-Langevin (ILL), University of British Columbia (UBC), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Independent Researcher, Coelho software, Finden Limited, Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), 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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Département de l'électricité et de l'hydrogène dans les transports (DEHT), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), ILL, Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de L'Energie Solaire (INES)

Subjects
inorganic chemicals, Materials science, Nanostructure, Renewable Energy, Sustainability and the Environment, Energy Engineering and Power Technology, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrocatalyst, 01 natural sciences, 7. Clean energy, Durability, 0104 chemical sciences, Catalysis, Fuel Technology, Chemical engineering, Chemistry (miscellaneous), Hydrogen fuel, Materials Chemistry, Energy transformation, Degradation (geology), 0210 nano-technology, Decoupling (electronics)
Abstract

International audience; Proliferation of hydrogen fuel cell systems is hindered by degradation of the platinum catalyst. Here, we provide a device level assessment of the catalyst degradation phenomena and its coupling to nanoscale hydration gradients, using advanced operando X-ray scattering tomography tailored for device-scale imaging. Gradients formed inside the fuel cell produce heterogeneous degradation of the catalyst nanostructure, which can be linked to the flow field design and water distribution in the cell. Striking differences in catalyst degradation are observed between operating fuel cell devices and the liquid cell routinely used for catalyst stability studies, highlighting the crucial impact of the complex operating environment on the catalyst degradation phenomena. This degradation knowledge gap accentuates the necessity of multimodal, in situ characterization of real devices when assessing the performance and durability of electrocatalysts, and more generally, electrochemically active phases used in energy conversion and storage technologies.

Published
2021
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25. Pristine and Modified Porous Membranes for Zinc Slurry–Air Flow Battery

Author

Mateusz L. Donten, Nadia El Kissi, Diego Milian, Fannie Alloin, Nak Heon Choi, Peter Fischer, Getachew Teklay Gebreslassie, Misgina Tilahun Tsehaye, Cristina Iojoiu, Vincent Martin, Jens Tübke, Matériaux Interfaces ELectrochimie (MIEL), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Fraunhofer Institute for Chemical Technology (Fraunhofer ICT), Fraunhofer (Fraunhofer-Gesellschaft), Karlsruhe Institute of Technology (KIT), Laboratoire Rhéologie et Procédés (LRP), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Electrochimie Interfaciale et Procédés (EIP), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-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 Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement no. 76528, European Project: 765289, European Project: 2011-0168, Université de Nantes (UN)-Aix Marseille Université (AMU)-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 Montpellier (ENSCM)-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)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), Univ. Grenoble Alpes, CNRS, Grenoble INP, LRP (LRP), and Université Grenoble Alpes [2016-2019] (UGA [2016-2019])

Subjects
Battery (electricity), Materials science, Pharmaceutical Science, chemistry.chemical_element, Organic chemistry, 02 engineering and technology, Electrolyte, Zinc, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Article, membrane coating, Analytical Chemistry, chemistry.chemical_compound, [SPI]Engineering Sciences [physics], Chemical engineering, QD241-441, Drug Discovery, zinc slurry–air flow battery, Ionic conductivity, Physical and Theoretical Chemistry, Ionomer, zincate crossover, UV irradiation, power density, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Flow battery, 0104 chemical sciences, Membrane, chemistry, Chemistry (miscellaneous), ddc:660, Molecular Medicine, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other, Zincate
Abstract

The membrane is a crucial component of Zn slurry–air flow battery since it provides ionic conductivity between the electrodes while avoiding the mixing of the two compartments. Herein, six commercial membranes (Cellophane™ 350PØØ, Zirfon®, Fumatech® PBI, Celgard® 3501, 3401 and 5550) were first characterized in terms of electrolyte uptake, ion conductivity and zincate ion crossover, and tested in Zn slurry–air flow battery. The peak power density of the battery employing the membranes was found to depend on the in-situ cell resistance. Among them, the cell using Celgard® 3501 membrane, with in-situ area resistance of 2 Ω cm2 at room temperature displayed the highest peak power density (90 mW cm−2). However, due to the porous nature of most of these membranes, a significant crossover of zincate ions was observed. To address this issue, an ion-selective ionomer containing modified poly(phenylene oxide) (PPO) and N-spirocyclic quaternary ammonium monomer was coated on a Celgard® 3501 membrane and crosslinked via UV irradiation (PPO-3.45 + 3501). Moreover, commercial FAA-3 solutions (FAA, Fumatech) were coated for comparison purpose. The successful impregnation of the membrane with the anion-exchange polymers was confirmed by SEM, FTIR and Hg porosimetry. The PPO-3.45 + 3501 membrane exhibited 18 times lower zincate ions crossover compared to that of the pristine membrane (5.2 × 10−13 vs. 9.2 × 10−12 m2 s−1). With low zincate ions crossover and a peak power density of 66 mW cm−2, the prepared membrane is a suitable candidate for rechargeable Zn slurry–air flow batteries.

Published
2021
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26. Formation of self-ordered oxide nanotubes layer on the equiatomic TiNbZrHfTa high entropy alloy and bioactivation procedure

Author

J.E. Berger, Alberto Moreira Jorge, Virginie Roche, G.H. Asato, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Materials science, Simulated body fluid, Alloy, Nucleation, Oxide, 02 engineering and technology, Substrate (electronics), engineering.material, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Ultimate tensile strength, Materials Chemistry, [CHIM]Chemical Sciences, Composite material, Polarization (electrochemistry), ComputingMilieux_MISCELLANEOUS, Mechanical Engineering, Metals and Alloys, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Mechanics of Materials, engineering, Surface modification, 0210 nano-technology
Abstract

The TiNbZrHfTa high entropy alloy was studied for its use as a base material for orthopedic implants. The alloy produced by arc melting contains only biocompatible elements and has an attractive combination of mechanical properties with a tensile strength of 1050 MPa and Young's modulus of 66 GPa. Surface modification techniques were carried out to bioactivate the alloy surface, ensuring better interaction between the implanted material and the human body. The first technique was the anodization in an organic electrolyte, containing F- ions in different potentials and time, obtaining the best condition at 10 V potential for 2 h at 20 °C, producing an ordered and adherent nanotubular morphology to the substrate. The second technique was precalcification. Using the alternation immersion method (AIM), the saturation and nucleation of Ca-P deposits were guaranteed, providing high deposition rates of hydroxyapatite (HAP) when immersed in simulated body fluid (SBF) solution. Structural characterizations were performed by XRD and XPS. Morphological analyses were performed by SEM and chemical semi-quantitative analyses by EDX. Corrosion resistance properties were performed through polarization and impedance curves. The TiNbZrHfTa high entropy alloy proved to be a competitive and attractive candidate in the research for new compositions to replace conventional alloys, having biocompatibility, high strength, and low Young's modulus, reducing stress shielding effects and showing good bioactivity characteristics through the surface modification techniques presented here.

Published
2021
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27. Synthesis of metallic nanoparticles for heterogeneous catalysis: Application to the Direct Borohydride Fuel Cell

Author

Gaël Maranzana, Léa Le Joncour, Fabrice Asonkeng, Marian Chatenet, Julien Proust, Jérôme Dillet, Sophie Didierjean, Guillaume Braesch, Thomas Maurer, Manuel François, Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Lumière, nanomatériaux et nanotechnologies (L2n), Université de Technologie de Troyes (UTT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Systèmes Mécaniques et d'Ingénierie Simultanée (LASMIS), Université de Technologie de Troyes (UTT), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and ANR-18-CE09-0003,INSOMNIA,Intégration de nanojauges pour le suivi optique de déformations(2018)

Subjects
FOS: Physical sciences, chemistry.chemical_element, Nanoparticle, Applied Physics (physics.app-ph), 010402 general chemistry, Borohydride, 7. Clean energy, 01 natural sciences, Catalysis, Metal, chemistry.chemical_compound, Direct Borohydride Fuel Cell (DBFC), Direct borohydride fuel cell, Platinum, Heterogeneous catalysis, 010405 organic chemistry, Chemistry, Process Chemistry and Technology, Propylene glycol methyl ether acetate, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, Physics - Applied Physics, 0104 chemical sciences, Borohydride Oxidation Reaction (BOR), Chemical engineering, visual_art, visual_art.visual_art_medium, Gold, chemical synthesis, Palladium
Abstract

Until now, the fabrication of electrocatalysts to guarantee long life of fuel cells and low consumption of noble metals remains a major challenge. The electrocatalysts based on metals or metal oxides which are used today are limited by the complexity of their synthesis processes and require several steps before depositing the catalysts on the substrate. Herein is described a chemical synthesis process that consists of a single-step synthesis and direct deposition of catalysts nanoparticles such as gold (Au), palladium (Pd) and platinum (Pt) in the thickness of a carbon-fibers-based porous transport layer (PTL). The synthesis process essentially consists of dissolving in the same PGMEA (Propylene glycol methyl ether acetate) solvent a metal precursor (HAuCl4 or PdNO2 or PtCl4) and a homopolymer PMMA (Polymethylmetacrylate), then the metal solution is deposited on the surface of the PTL after cleaning. Special emphasis is made on Pt-based materials. The obtained PTL-supported nanoparticles were firstly characterized by scanning electron microscopy (SEM) to evaluate their morphology, and then X-Ray diffraction (XRD) to observe the crystal phases. To validate the methodology, Pt-coated PTL materials have been used as anode for the borohydride oxidation reaction (BOR) in a direct borohydride fuel cell (DBFC) and compared to a state-of-the-art nickel electrode. There is an optimum loading of platinum (below 0.16 mg Pt / cm2) which constitutes the best compromise between power density and faradic efficiency for the borohydride oxidation reaction (BOR). Thanks to this low Pt loading, hydrogen evolved during the anodic reaction is completely valorized. These electrodes combine the advantages of high-performance with a very low metal loading, hence lowering materials’cost.

Published
2021
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28. Towards the understanding of transport limitations in a proton-exchange membrane fuel cell catalyst layer: Performing agglomerate scale direct numerical simulations on electron-microscopy-based geometries

Author

Y. Bultel, M. Barreiros Salvado, Laure Guetaz, T. David, Mathias Gerard, Pascal Schott, Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)

Subjects
Materials science, Renewable Energy, Sustainability and the Environment, Scanning electron microscope, Energy Engineering and Power Technology, Proton exchange membrane fuel cell, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Focused ion beam, Dark field microscopy, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Chemical physics, Nafion, Phase (matter), Scanning transmission electron microscopy, [CHIM]Chemical Sciences, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, 0210 nano-technology, High-resolution transmission electron microscopy, ComputingMilieux_MISCELLANEOUS
Abstract

Improving the cathode catalyst layer design requires understanding the sources of transport limitations in proton-exchange membrane fuel cells. For the purpose, a framework consisting on an electron microscopy characterization setup in couple with a numerical modeling software is proposed. The latter integrates high-performing geometry building capabilities which ensure full phase discretization (carbon, platinum, ionomer and pore phase) and freedom when designing the structure morphology and meshing. The 3D structure of the carbon phase is extracted from a focused ion beam scanning electron microscopy analysis having a 2 nm isotropic resolution. The platinum phase is built according to a nanoparticle size histogram determined from high angle annular dark field scanning transmission electron microscopy images. To add the ionomer phase, the thickness of the layer is measured on high resolution transmission electron microscopy images. The multi-physics model includes gas transport in the pores, and gas and ionic transport in the Nafion. A 4-step reaction mechanism is used to solve the electrochemistry. Numerical simulations are performed on two catalyst layer portions. The results show that structural heterogeneities can deeply impact performance. Such impact is mainly linked to oxygen diffusion limitations through the Nafion film and, to a certain extent, to interparticle competition effects.

Published
2021
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29. Dimensionless approach of a polymer electrolyte membrane water electrolysis: Advanced analytical modelling

Author

Maha Rhandi, Brigitte Grondin-Perez, Jude O. Majasan, Jonathan Deseure, Farid Aubras, Jean-Pierre Chabriat, Miloud Bessafi, Amangoua Jean-Jacques Kadjo, Florence Druart, Laboratoire d'Energétique, d'Electronique et Procédés (LE2P), Université de La Réunion (UR), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Electrochemical Innovation Lab, Department of Chemical Engineering, University College of London [London] (UCL), and The authors would like to acknowledge the Regional Council of La Reunion, the local management authority for the European Regional Development Fund (ERDF), and the SIDELEC trough the SPACE project, GRANT N D2018026063/GURDTI/SN/SU/EM/MI.

Subjects
Materials science, Hydrogen, Energy Engineering and Power Technology, Thermodynamics, Proton exchange membrane fuel cell, chemistry.chemical_element, 02 engineering and technology, Electrolyte, PEM water electrolysis, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Dimensionless model, Two-phase flow characterisation, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, Hydrogen production, [PHYS]Physics [physics], Water transport, Electrolysis of water, Renewable Energy, Sustainability and the Environment, Closed-form solution, 021001 nanoscience & nanotechnology, Thiele modulus, 6. Clean water, 0104 chemical sciences, chemistry, 0210 nano-technology, Dimensionless quantity
Abstract

The water electrolysis appears as a sustainable solution for hydrogen production. The proton exchange membrane electrolyzers (PEM-E) play an increasingly important role in the development of hydrogen technology. Fast analysis of PEM-E efficiency using a mathematical approach is an effective tool for the improvement of these devices. This work presents a closed-form solution of single cell PEM-E modelling. The approach considers charge and mass transport balances. The one-dimensional study focuses on the anodic and the cathodic catalyst layer and the membrane using only dimensionless parameters. The analytical model allows to describe the water management as a function of pressure gradient and current density using a dimensionless ratio of water transport process ( β m , ). This model is endorsed by experimental data. Dimensionless parameters like Thiele modulus ( β a , c ) or Wagner number ( ω a , C ) are reached using numerical optimization methods. Changing values of dimensionless numbers, allow the observation of the impact of the two-phase flow regimes on the electrochemical performances.

Published
2021
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30. Experimental and theoretical investigation of Li-ion battery active materials properties: Application to a graphite/Ni0.6Mn0.2Co0.2O2 system

Author

Jean-Michel Réty, Oumaima Chaouachi, M. Chandesris, Yann Bultel, Sylvie Genies, Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)

Subjects
Battery (electricity), Materials science, Fundamental thermodynamic relation, General Chemical Engineering, Thermodynamics, Exchange current density, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, Lithium-ion battery, 0104 chemical sciences, Dielectric spectroscopy, chemistry, Electrochemistry, [CHIM]Chemical Sciences, Lithium, Graphite, 0210 nano-technology, Material properties, ComputingMilieux_MISCELLANEOUS
Abstract

The knowledge of active materials properties and their evolution with aging is crucial to simulate and predict with a high reliability the electrochemical performance of lithium-ion batteries. In view of developing more accurate physics-based Lithium Ion Battery (LIB) models, this paper aims to present a consistent framework, including both experiments and theory, in order to retrieve the active material properties of commonly used electrodes made of graphite at the negative and Ni0.6Mn0.2Co0.2O2 (NMC 622) at the positive, as function of the active materials stoichiometry. To measure the equilibrium potential and the solid diffusion coefficient, Galvanostatic Intermittent Titration Technique (GITT) measurements were used. Electrochemical impedance spectroscopy (EIS) measurements with reference electrodes were performed to determine the exchange current density using the transmission line model. The measured stoichiometry dependence of these three active material properties has been further analyzed, based on thermodynamic considerations. For the positive material, a model is proposed highlighting the non-ideal behavior of lithium inside the host material. The thermodynamic relations available in the literature are not directly transposable to the Ni0.6Mn0.2Co0.2O2 material, suggesting the necessity to account for supplementary terms. Nevertheless, the proposed stoichiometry dependent laws determined with the same stoichiometry definition go already beyond most reported values for the Ni0.6Mn0.2Co0.2O2 and can be used to increase the predictability of multi-physics lithium-ion battery models.

Published
2021
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31. Towards comprehensive understanding of proton-exchange membrane fuel cells using high energy X-rays

Author

Frédéric Maillard, Tim Wiegmann, Olaf M. Magnussen, Jakub Drnec, Laetitia Dubau, Isaac Martens, Raphaël Chattot, Timo Fuchs, European Synchroton Radiation Facility [Grenoble] (ESRF), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institut für Experimentelle und Angewandte Physik [Kiel] (IEAP), Christian-Albrechts-Universität zu Kiel (CAU), ANR-19-ENER-0008,BRIDGE,Vers l'intégration de catalyseurs performants dans des électrodes de pile à combustible efficaces(2019), and ANR-10-LABX-0044,CEMAM,Center of Excellence in Multifunctional Architectured Materials(2010)

Subjects
High energy, Materials science, high energy X-rays, Materials Science (miscellaneous), Proton exchange membrane fuel cell, 02 engineering and technology, fuel cells, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Effective energy, Hydrogen economy, Materials Chemistry, Power output, Energy, catalysis, business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Engineering physics, 0104 chemical sciences, General Energy, High-energy X-rays, Fuel cells, 0210 nano-technology, business
Abstract

For a future hydrogen economy, the development of cost effective energy conversion devices is a key issue. In this perspective, we discuss the use of high energy x-rays for obtaining comprehensive insights into the complex processes which occur inside such devices, focusing on proton exchange membrane fuel cells. This probe enables structural characterisation under operating conditions on all relevant length scales, from the atomic-scale interfaces to complete stacks. This opens up possibilities to go beyond characterisation of the isolated components, towards an understanding of their interactions in the full system which determine the power output, efficiency and degradation pathways in operational devices.

Published
2021
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32. Characterization of Optimized TiO2 Nanotubes Morphology for Medical Implants: Biological Activity and Corrosion Resistance

Author

Ricardo P. Nogueira, Virginie Roche, Alberto Moreira Jorge Junior, Jose Deuzimar Uchoa, Anderson Oliveira Lobo, Fernanda Roberta Marciano, Luana Marotta Reis de Vasconcellos, Fanny Hilario, Gabriela de Fátima Santana-Melo, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Khalifa Univ Sci & Technol, Univ Grenoble Alpes, Fed Inst Educ Sci & Technol Piaui, UFPI Fed Univ Piaui, Universidade Estadual Paulista (Unesp), Univ Fed Piaui, and Universidade Federal de São Carlos (UFSCar)

Subjects
commercially pure titanium, Materials science, Cell Survival, Simulated body fluid, Biophysics, Pharmaceutical Science, Bioengineering, 02 engineering and technology, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, Corrosion, Biomaterials, Barrier layer, Electrolytes, International Journal of Nanomedicine, Cell Line, Tumor, Drug Discovery, Cell Adhesion, TiO2 nanotubes, Humans, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS, Original Research, Titanium, Nanotubes, Organic Chemistry, General Medicine, Prostheses and Implants, 021001 nanoscience & nanotechnology, Alkaline Phosphatase, 0104 chemical sciences, Amorphous solid, Chemical engineering, Rutile, bioactivity, Wettability, Surface modification, 0210 nano-technology, surface modification
Abstract

Ricardo Pereira Nogueira,1,2 Jose Deuzimar Uchoa,3,4 Fanny Hilario,2 Gabriela de Fátima Santana-Melo,5 Luana Marotta Reis de Vasconcellos,5 Fernanda Roberta Marciano,6 Virginie Roche,2 Alberto Moreira Jorge Junior,2,7 Anderson Oliveira Lobo4 1Chemical Engineering Department, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates; 2Université Grenoble Alpes, Université Savoie Mont Blanc, CNRS, GrenobleINP*LEPMI, Grenoble 38000, France; 3Federal Institute of Education, Science and Technology of Piauí, Teresina 64053-390, Brazil; 4Interdisciplinary Laboratory for Advanced Materials, BioMatLab Group, Materials Science and Engineering Graduate Program, UFPI – Federal University of Piaui, Teresina 64049-550 Brazil; 5Department of Bioscience and Oral Diagnosis, Institute of Science and Technology, Sao Paulo State University, Sao José dos Campos 12245-000, Brazil; 6Department of Physics, Federal University of Piaui, Teresina PI 64049-550 Brazil; 7Department of Materials Engineering, Federal University of São Carlos, São Carlos 13565-905, BrazilCorrespondence: Anderson Oliveira LoboCampus Universitário Ministro Petrônio Portella, Av. Universitária, s/n, Centro de Tecnologia, Laboratório Interdisciplinar de Materiais Avançados, Ininga, Teresina, PI 64049-550, BrazilTel +55 86 32371057Email lobo@ufpi.edu.brBackground: Nanostructured surface modifications of Ti-based biomaterials are moving up from a highly-promising to a successfully-implemented approach to developing safe and reliable implants.Methods: The study’s main objective is to help consolidate the knowledge and identify the more suitable experimental strategies related to TiO2 nanotubes-modified surfaces. In this sense, it proposes the thorough investigation of two optimized nanotubes morphologies in terms of their biological activity (cell cytotoxicity, alkaline phosphatase activity, alizarin red mineralization test, and cellular adhesion) and their electrochemical behavior in simulated body fluid (SBF) electrolyte. Layers of small-short and large-long nanotubes were prepared and investigated in their amorphous and crystallized states and compared to non-anodized samples.Results: Results show that much more than the surface area development associated with the nanotubes’ growth; it is the heat treatment-induced change from amorphous to crystalline anatase-rutile structures that ensure enhanced biological activity coupled to high corrosion resistance.Conclusion: Compared to both non-anodized and amorphous nanotubes layers, the crystallized nano-structures’ outstanding bioactivity was related to the remarkable increase in their hydrophilic behavior, while the enhanced electrochemical stability was ascribed to the thickening of the dense rutile barrier layer at the Ti surface beneath the nanotubes.Keywords: surface modification, TiO2 nanotubes, commercially pure titanium, bioactivity

Published
2021
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33. Effect of hydrogen pick-up on the fatigue behavior of the β-type Ti-12Mo-6Zr-2Fe alloy with ω-nanoprecipitation

Author

Alberto Moreira Jorge, Danieli Aparecida Pereira Reis, Brenda Juliet Martins Freitas, Leonardo Contri Campanelli, Claudemiro Bolfarini, Cesar Adolfo Escobar Claros, Science et Ingénierie des Matériaux et Procédés (SIMaP), Institut de Chimie du CNRS (INC)-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), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )

Subjects
Materials science, Precipitation (chemistry), Hydride, Mechanical Engineering, Alloy, 02 engineering and technology, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Fatigue limit, Isotropic etching, Nanocrystalline material, 0104 chemical sciences, Mechanics of Materials, Ultimate tensile strength, engineering, [CHIM]Chemical Sciences, General Materials Science, Grain boundary, Composite material, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

The metastable β-type Ti-12Mo-6Zr-2Fe alloy was subjected to an assessment of its fatigue mechanical behavior. Promising tensile and fatigue properties were obtained when the alloy was solution treated and quenched, because nanocrystalline particles of ω phase were formed throughout the β matrix. When the material was subjected to a protocol of chemical etching and a subsequent surface polishing, the fatigue limit decreased significantly as a result of H pick-up, although the tensile properties were not changed. The increase of the local H concentration caused the precipitation of fine hydrides at high-energy grain boundaries. Fatigue crack initiation changed to a subsurface mode induced by the cleavage of hydride precipitates.

Published
2021
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34. Oxygen Evolution Reaction Activity and Stability Benchmarks for Supported and Unsupported IrOx Electrocatalysts

Author

Vincent Martin, Fabio Henrique Barros de Lima, Thierry Encinas, Frédéric Maillard, Marco Faustini, Camila Daiane Ferreira da Silva, Sofyane Abbou, Sara Cavaliere, Bruno Gilles, Ignacio Jiménez-Morales, Laurent Piccolo, Kavita Kumar, Jennifer Peron, Laetitia Dubau, Deborah J. Jones, Jacques Rozière, Christian Beauger, Raphaël Chattot, Fabien Claudel, Lluis Sola-Hernandez, Universidade de São Paulo (USP), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), 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), Centre Procédés, Énergies Renouvelables, Systèmes Énergétiques (PERSEE), MINES ParisTech - École nationale supérieure des mines de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), 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 de Paris (UP), Science et Ingénierie des Matériaux et Procédés (SIMaP), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Consortium des Moyens Technologiques Communs (CMTC), Institut National Polytechnique de Grenoble (INPG), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR, ANR-17-CE05-0033,MOISE,Oxydes métalliques comme Support d'iridium nano faiblement chargé pour une électrolyse de l'eau compétitive(2017), and ANR-10-LABX-0044,CEMAM,Center of Excellence in Multifunctional Architectured Materials(2010)

Subjects
Materials science, doped tin oxide, Nanoparticle, chemistry.chemical_element, Electrolyte, 010402 general chemistry, Electrochemistry, 01 natural sciences, 7. Clean energy, Catalysis, S-number, 010405 organic chemistry, Oxygen evolution, General Chemistry, Carbon black, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, proton exchange membrane water electrolyzer, iridium oxide nanoparticles, Nanomaterial-based catalyst, 0104 chemical sciences, Chemical engineering, chemistry, 13. Climate action, oxygen evolution reaction, ELETROCATÁLISE, Tin
Abstract

International audience; Advanced materials are needed to meet the requirements of devices designed for harvesting and storing renewable electricity. In particular, polymer electrolyte membrane water electrolyzers (PEMWEs) could benefit from a reduction in the size of the iridium oxide (IrO x) particles used to electrocatalyze the sluggish oxygen evolution reaction (OER). To verify the validity of this approach, we built a library of 18 supported and unsupported IrO x catalysts and established their stability number (S-number) values using inductively coupled plasma mass spectrometry and electrochemistry. Our results provide quantitative evidence that (i) supported IrO x nanocatalysts are more active toward the OER but less stable than unsupported micrometer-sized catalysts, for example, commercial IrO 2 or porous IrO x microparticles; (ii) tantalum-doped tin oxides (TaTO) used as supports for IrO x nanoparticles are more stable than antimony-doped tin oxides (ATO) and carbon black (Vulcan XC72); (iii) thermal annealing under air atmosphere yields depreciated OER activity but enhanced stability; (iv) the beneficial effect of thermal annealing holds both for micro-and nano-IrO x particles and leads to 1 order of magnitude lower Ir atom dissolution rate with respect to nonannealed catalysts; (v) the best compromise between OER activity and stability was obtained for unsupported porous IrO x microparticles after thermal annealing under air at 450°C. These insights provide guidance on which material classes and strategies are the most likely to increase sustainably the OER efficiency while contributing to diminish the cost of PEMWE devices.

Published
2021
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35. Fe-N-C Electrocatalysts' Durability: Effects of Single Atoms' Mobility and Clustering

Author

Michel Mermoux, Frédéric Maillard, Kavita Kumar, Plamen Atanassov, Xiaoyan Li, Yechuan Chen, Xingxu Yan, Xiaoqing Pan, Yuanchao Liu, Laetitia Dubau, Tristan Asset, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), University of California [Irvine] (UCI), University of California, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Matériaux Interfaces ELectrochimie (MIEL), and ANR-19-CE05-0039,ANIMA,Aérogels de carbone poreux dopés à l'azote et avec des métaux abondants pour des assemblages membrane-électrodes efficaces et durables(2019)

Subjects
Materials science, 010405 organic chemistry, chemistry.chemical_element, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, Platinum group, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Durability, Catalysis, 3. Good health, 0104 chemical sciences, chemistry, Chemical engineering, Cathode material, Atom, Metal nanoparticles, Carbon, ComputingMilieux_MISCELLANEOUS
Abstract

Atomically dispersed (or single atom) iron–nitrogen–carbon (Fe–N–C) catalysts are promising alternatives to platinum group metal nanoparticles supported on dispersed carbon as a cathode material in...

Published
2020
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36. Ammonium chloride effects on bismuth electrodeposition in a choline chloride-urea deep eutectic solvent

Author

N. Benbrahim, Eric Chainet, Salem Boudinar, A. Kadri, Jean-Claude Leprêtre, Youcef Karar, Laboratoire de physique et de chimie des matériaux [Tizi-Ouzou] (LPCM), Université Mouloud Mammeri [Tizi Ouzou] (UMMTO), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Matériaux Interfaces ELectrochimie (MIEL)

Subjects
inorganic chemicals, Materials science, General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Bismuth, chemistry.chemical_compound, law, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Electrochemistry, Ammonium, Crystallization, food and beverages, [CHIM.MATE]Chemical Sciences/Material chemistry, Chronoamperometry, 021001 nanoscience & nanotechnology, digestive system diseases, 0104 chemical sciences, Deep eutectic solvent, chemistry, Melting point, Ammonium chloride, 0210 nano-technology, Choline chloride
Abstract

International audience; The ammonium chloride effect on bismuth electrodeposition from choline chloride-urea deep eutectic solvent (DES) was investigated. Spectroscopic and thermal studies were performed on the latter in order to understand whether the addition of ammonium chloride affects the DES behavior; the results of the thermal study do not indicate any significant change except a small shift in the melting point of the DES when adding the ammonium salt (~+3 °C) and the modification of a cold crystallization peaks at low scan rate. The electrochemical behavior of bismuth was then studied by cyclic voltammetry in the deep eutectic solvent with different NH4Cl content. Bismuth electrocrystallization was studied by chronoamperometry which has shown that the bismuth electrodeposition in studied conditions evolves with a three-dimensional progressive nucleation. SEM images show that grain size of bismuth deposits decreases while adopting a well-defined geometry as ammonium salt concentration increases. EDS analysis confirms that pure bismuth thin films were obtained and X-Ray diffraction indicates that the bismuth growth follows a preferential orientation along the (012) reticular plane.

Published
2020
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37. A Comparison of Cobalt and Platinum Extraction in Hydrophobic and Hydrophilic Ionic Liquids: Implication for Proton Exchange Membrane Fuel Cell Recycling

Author

Lenka Svecova, Matthieu Gras, Vijetha Mogilireddy, Isabelle Billard, Nicolas Papaiconomou, Lucien Duclos, Eric Chainet, Nicolas Schaeffer, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Closed loop, General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, Proton exchange membrane fuel cell, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Chloride, chemistry.chemical_compound, medicine, Environmental Chemistry, Fuel cells, Process evaluation 16 17, Aqueous solution, Renewable Energy, Sustainability and the Environment, Aqueous two-phase system, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Ionic liquids, Solvent, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry, Ionic liquid, Metal ion separation, 15 Recycling, 0210 nano-technology, Platinum, Cobalt, [CHIM.RADIO]Chemical Sciences/Radiochemistry, medicine.drug
Abstract

International audience; 18 Starting from a real Proton Exchange Membrane Fuel Cell (PEMFC) leachate, separation of the 19 strategic metals platinum(IV) and cobalt(II) was carried out using two distinct strategies applying ionic 20 liquids (ILs), either via solvent extraction (SX) or acidic aqueous biphasic system (AcABS). The 21 versatility of ILs and their ability to provide original solutions to common issues in the field of used 22 device recycling is illustrated, with both approaches critically compared. The highly hydrophobic 23 tetradecylpyridinium bis(trifluoromethanesulfonyl)imide ([C 14 pyr][NTf 2 ]) was synthesized and applied 24 to the separation of Pt/Co. This solvent was able to selectively extract over 98% of Pt(IV) from the 25 PEMFC leachate in one step while leaving Co(II) in the aqueous phase and exhibited the highest 26 reported partition of Pt(IV) in a [NTf 2 ]-based IL. In a second approach, the AcABS based on the fully 27 water-miscible tributyltetradecylphosphonium chloride ([P 44414 ]Cl), HCl and water, is compatible with 28 the concentrated nature of the leachate and extracts both platinum(IV) and cobalt(II) quantitatively. In 29 a second stage, a selective precipitation step enabled the recovery of platinum(IV) in the form of an 30 organometallic complex whilst leaving the co-extracted cobalt(II) in solution. This work represents the 31 2 first utilization of an AcABS for the recycling of a real waste technological object. These two different 32 types of ILs in both cases resulted in an efficient separation of Pt(IV) from Co(II), using two very 33 different pathways. The merit and transferability of each approach is critically compared, and 34 suggestions are made as to the suitable condition range for each technique. 35 36

Published
2020
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38. Uncommon biphasic behaviour induced by very high metal ion concentrations in HCl/H 2 O/[P 44414 ]Cl and HCl/H 2 O/PEG-600 systems

Author

Isabelle Billard, Victor Maia Fernandes, Ismaël Guillotte, Jorge F. B. Pereira, Jérôme Cognard, Eris Sinoimeri, Lenka Svecova, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
chemistry.chemical_classification, Binodal, Aqueous solution, Metal ions in aqueous solution, Extraction (chemistry), Inorganic chemistry, General Physics and Astronomy, Hydrochloric acid, 02 engineering and technology, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Metal, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry.chemical_compound, chemistry, visual_art, Ionic liquid, visual_art.visual_art_medium, Physical and Theoretical Chemistry, 0210 nano-technology, [CHIM.RADIO]Chemical Sciences/Radiochemistry
Abstract

International audience; In this work, the important role played by metal ions such as Fe(II/III), Cr(III) and Ni(II) in the formation and binodal behaviour of aqueous biphasic systems (ABS) composed of HCl and the ionic liquid, [P44414]Cl, or the polymer, PEG-600, is investigated. The concentration of metal ions used in this work exceeds several g/L for an industrial foreseen application. Experiments have also been carried out by varying the concentration of metal ions at different temperatures. Fe exhibits a totally different behaviour compared to Ni and Cr. In particular, the binodal curves in presence of the ionic liquid are far from the classical curves found in the literature, displaying an onion-shape form, while for Ni and Cr, the curves follow the classical trend. When any of the three metal ions is mixed with the polymer and HCl medium, only Fe(III) induces a biphasic system. Insights into the chemical driving forces at work are discussed.Introduction In recent years, neutral Aqueous Biphasic Systems (ABS), composed of different polymer-polymer, polymer-salt or salt-salt combinations, plus water as the main protagonist, have been taken into consideration to selectively extract metal ions. In particular, the use of the [P44414]Cl (tri-butyl tetradecyl phosphonium chloride) ionic liquid (IL) or of the polyethene glycol (PEG) polymer for metal extraction has already been the subject of several papers. 1-6 The use of these compounds, more appropriately called biphasic inducers in these classical ABS, helps to make the process eco-sustainable. The [P44414]Cl hydrophilic ionic liquid (i) is less toxic than the respective hydrophobic IL 7 , (ii) can be used in much lower quantities than organic volatile solvents and (iii) the extraction kinetics is favored by its low viscosity. In regards to the PEG, this is an inexpensive, nontoxic, non-flammable compound which is commercially available in very large quantities. These systems are intrinsically much eco-friendlier than the classical liquid-liquid systems where organic solvents are used as main components and could thus be favorably considered by the industry. However, in order to comply with any industrial demand, extraction should proceed from highly loaded wastes, which is currently very rarely the case in the literature. Furthermore, most industrial wastes are highly acidic, which is not compatible with the most classical ABSs. Therefore, in the first step, we took advantage of the recently described Acidic Aqueous Biphasic Systems (AcABS) 8 loaded with very high concentrations of either Cr, Ni or Fe to perform fundamental studies in view of potential industrial applications. In this work, aqueous biphasic systems (ABS) are formed from solutions containing a single metal element, HCl as the acid, and using either [P44414]Cl or PEG as biphasic inducer. We focused on the influence of the metal, in particular on the contribution coming from the type of metal used and on its concentration. Furthermore, the influence of temperature has been taken into consideration for industrial needs. Finally, we reviewed past literature which proposed some possible explanations and we discussed these under the light of our experimental results. Experimental Section Chemicals Polyethene glycol with an average molecular weight of 600 (abbreviated as PEG-600) was acquired from Acros Organics. The ionic liquid tributyl tetradecyl phosphonium chloride, [P44414]Cl, was acquired from Interchim (Montluçon, France). The declared purity was > 95%. Some basic physicochemical properties of PEG-600 are reported in the supplementary materials. The hydrochloric acid, HCl, (37 wt% = 12 mol/L, in water) was acquired from Sigma-Aldrich. The following hydrated salts have been used: NiCl2.6H2O pure at 98% acquired from Rectapur, CrCl3.6H2O pure at 98% acquired from Fluka, FeCl2.4H2O pure at 98% and FeCl3.6H2O pure at 99% were acquired from Merck. All the chemicals were used without further purification. The water used in all experiments was passed through a Milli-Q apparatus purification system commercialized by Merck (18MΩ). AAS (Atomic Absorption Spectroscopy) single element standard solutions (1000 mg/L) were acquired from Perkin Elmer for Cr and from Chem-Lab for Fe and Ni. Sample preparation

Published
2020
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39. Advances in tailoring the water content in porous carbon aerogels using RT-pulsed fluorination

Author

Sandrine Berthon-Fabry, Marc Dubois, Yasser Ahmad, Guillaume Monier, Marian Chatenet, Katia Guérin, Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institut de Chimie de Clermont-Ferrand - Clermont Auvergne (ICCF), Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA)-Sigma CLERMONT (Sigma CLERMONT), Centre Procédés, Énergies Renouvelables, Systèmes Énergétiques (PERSEE), Mines Paris - PSL (École nationale supérieure des mines de Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Electrochimie Interfaciale et Procédés (EIP), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Institut de Chimie de Clermont-Ferrand (ICCF), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA)-Institut national polytechnique Clermont Auvergne (INP Clermont Auvergne), Université Clermont Auvergne (UCA)-Université Clermont Auvergne (UCA), Sigma CLERMONT (Sigma CLERMONT)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), MINES ParisTech - École nationale supérieure des mines de Paris, and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)

Subjects
010405 organic chemistry, Chemistry, Organic Chemistry, chemistry.chemical_element, Aerogel, [CHIM.CATA]Chemical Sciences/Catalysis, Conductivity, 010402 general chemistry, 01 natural sciences, Biochemistry, 0104 chemical sciences, Inorganic Chemistry, Chemical engineering, Covalent bond, Fluorine, Environmental Chemistry, Texture (crystalline), Physical and Theoretical Chemistry, Porosity, Carbon, Water content, ComputingMilieux_MISCELLANEOUS
Abstract

The present work introduces a safe and efficient fluorination method, called RT-pulsed fluorination, proceeding under pure fluorine gas. The RT-pulsed fluorination enables to modify the surface chemistry of carbon aerogels (CAs), materials which suffer from water trapping into their porosity and their low degree of graphitization, hence limiting their application. This new fluorination route was developed to reach several goals, such as preventing the generation of structural defects, maintaining the tailored porous texture of the aerogel, favoring covalent C–F bonding without promoting CF2 and CF3 groups, and repulsing the water trapping into the porosity. The impact of the RT-pulsed fluorination on the conductivity will be also discussed.

Published
2020
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40. Carbon-Supported PtNi Nanocrystals for Alkaline Oxygen Reduction and Evolution Reactions: Electrochemical Activity and Durability upon Accelerated Stress Tests

Author

Melina Zysler, Marian Chatenet, Meital Shviro, Victor Shokhen, David Zitoun, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Materials science, Oxygen evolution reaction, 020209 energy, Alloy, Energy Engineering and Power Technology, chemistry.chemical_element, Nanoparticle, 02 engineering and technology, engineering.material, 010402 general chemistry, Electrocatalyst, Electrochemistry, 01 natural sciences, 7. Clean energy, Durability, Catalysis, Oxygen reduction reaction, Platinum nickel octahedral, Carbon-supported catalyst, 0202 electrical engineering, electronic engineering, information engineering, Materials Chemistry, Chemical Engineering (miscellaneous), Electrical and Electronic Engineering, Alkaline fuel cells, Alkaline water electrolysis, Oxygen evolution, [CHIM.CATA]Chemical Sciences/Catalysis, 0104 chemical sciences, chemistry, Chemical engineering, 13. Climate action, Identical-location transmission electron microscopy (IL-TEM) 2, ddc:540, engineering, Alkaline electrolyzer, Carbon
Abstract

International audience; PtNi is amongst the most active electrocatalyst for the oxygen reduction reaction, but its stability in operation is uncertain. Intuitively, alkaline environments lead to milder degradations than acidic ones, although carbon-supported Pt-group metal nanoparticles are particularly degraded even in dilute alkaline electrolytes. To date, PtNi catalysts durability has not been characterized for alkaline oxygen reduction and evolution reactions (ORR and OER). Herein, carbon-supported shape controlled PtNi catalysts were compared in terms of activity and durability during alkaline ORR and OER. The PtNi catalysts are shape-controlled Pt-rich alloy, Ni-rich alloy, and Pt core/Ni shell (Pt@Ni) synthesized on Vulcan XC72R carbon. Their morphology and composition were evaluated by identical-location transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray diffraction pre and post accelerated stress test. Compared to Pt/C and Ni/C benchmark catalysts, the core-shell and Ni-rich alloy catalysts gave high and stable OER activities. After accelerated stress test, the catalysts show two features which are believed to play a major role in the durability: a Ni-enrichment at the nanoparticles' surface and an improved attachment of the catalyst to the carbon support.

Published
2020
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41. Building Practical Descriptors for Defect Engineering of Electrocatalytic Materials

Author

Pierre Bordet, Isaac Martens, Laetitia Dubau, Raphaël Chattot, Frédéric Maillard, Jakub Drnec, European Synchrotron Radiation Facility (ESRF), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Matériaux, Rayonnements, Structure (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 ), and 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 )

Subjects
Materials science, Defect engineering, Nanotechnology, 02 engineering and technology, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Catalysis, 0104 chemical sciences, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2020
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42. Evaluation of carbon-supported palladium electrocatalysts for the borohydride oxidation reaction in conditions relevant to fuel cell operation

Author

Clémence Lafforgue, Karen E. Swider-Lyons, Robert W. Atkinson, Marian Chatenet, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), and Naval Research Laboratory, Washington, DC, United States

Subjects
Materials science, General Chemical Engineering, Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Borohydride, Electrocatalyst, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Sodium borohydride, chemistry.chemical_compound, chemistry, Standard electrode potential, Electrochemistry, Reversible hydrogen electrode, [CHIM]Chemical Sciences, Rotating disk electrode, Cyclic voltammetry, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Palladium
Abstract

Direct borohydride fuel cells (DBFCs) take advantage of sodium borohydride (NaBH4) fuel to exhibit high theoretical energy density and a high theoretical cell voltage. Despite these promises, the borohydride electrooxidation reaction (BOR) at the anode is highly complex, has numerous byproducts, and remains poorly understood (and even poorly studied) on many electrocatalysts (in practice, only the behavior of Pt and Au is well characterized), especially at high NaBH4 concentrations and high temperature, i.e. in typical DBFC operating conditions. We study here how high fuel concentration and high temperature impact the BOR on carbon-supported Pd-based electrocatalysts. Four carbon-supported palladium electrocatalysts (Pd/C) with Pd weight fractions of 22–53% are studied for the BOR by cyclic voltammetry with a rotating disk electrode for three NaBH4 concentrations (5, 50 and 500 mM) in 1 M NaOH at T = 60 °C. To ensure accurate comparison of the electrocatalyst BOR activities, the electrochemical surface area of the Pd nanoparticles (NPs) are characterized by palladium oxide reduction, CO-adsorption and transmission electron microscopy. BOR activity markers are proposed to compare the various electrode materials, based on the activity obtained at three electrode potentials (0, 0.2 and 0.5 V vs. the reversible hydrogen electrode (RHE)) and enable clear comparison between them and state-of-the-art electrocatalyst Pt/C. In conditions close to DBFC operating conditions, the BOR can start at very low potentials on Pd/C electrocatalysts (−0.23 V vs. RHE), but the BOR kinetics is very slow for 5 and 50 mM NaBH4 in comparison to Pt/C, owing, at least in part, to poisoning of the catalytic surface by byproducts of the BOR.

Published
2020
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43. Nickel 3D Structures Enhanced by Electrodeposition of Nickel Nanoparticles as High Performance Anodes for Direct Borohydride Fuel Cells

Author

Gaël Maranzana, Guillaume Braesch, Alexandr G. Oshchepkov, Fabrice Asonkeng, Thomas Maurer, Elena R. Savinova, Marian Chatenet, Antoine Bonnefont, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences (SB RAS), Lumière, nanomatériaux et nanotechnologies (L2n), Institut Charles Delaunay (ICD), Université de Technologie de Troyes (UTT)-Centre National de la Recherche Scientifique (CNRS)-Université de Technologie de Troyes (UTT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), VU VAN, Jean-Baptiste, and ANR-16-CE05-0009,MobiDiC,Pile à combustible directe à borohydrure pour applications mobiles(2016)

Subjects
Materials science, [SPI.OPTI] Engineering Sciences [physics]/Optics / Photonic, Nanoparticle, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Borohydride, 7. Clean energy, 01 natural sciences, Catalysis, 0104 chemical sciences, Anode, chemistry.chemical_compound, Nickel, chemistry, Chemical engineering, Direct borohydride fuel cell, Electrochemistry, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Fuel cells, 0210 nano-technology
Abstract

International audience; Direct borohydride fuel cell (DBFC) is a promising technology to power portable and mobile devices thanks to their high theoretical voltage and good energy density. Carbon‐supported electrodeposited nickel‐metal catalysts (NiED/C) exhibit fast kinetics for the borohydride oxidation reaction (BOR). One key is to deposit nickel‐metal on sufficiently open structures to make electrodes compatible with fast mass‐transfer, so as to further optimize the fuel cell performance. To that goal, Ni foams (NFM) or felts (NFT) can be used. Being inherently surface‐oxidized (passivated) and of too low developed area, these supports were enhanced by both oxides removal/depassivation (using electro‐assisted (or not) acid etching) and nickel electrodeposition, in order to exhibit the combined properties of fast diffusion medium and high‐surface area resulting in the highly‐active catalysts. After such enhancement, NiED/NFT shows superior performance in the BOR compared to carbon‐supported Ni catalysts. To make a fair comparison with PGM, Pt catalysts supported on open carbon structures were also studied and presented slightly smaller performance than the NiED/NFT electrodes, in particular in terms of open‐circuit potential and current density at high cell voltage.

Published
2020
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44. Sulfur-based electrode using a polyelectrolyte binder studied via coupled in situ synchrotron X-ray diffraction and tomography

Author

Fannie Alloin, Pierre-Xavier Thivel, Quentin Lemarié, Hassane Idrissi, Lionel Roué, Eric Maire, Énergie Matériaux Télécommunications - INRS (EMT-INRS), Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM), Matériaux, ingénierie et science [Villeurbanne] (MATEIS), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Matériaux Interfaces ELectrochimie (MIEL), and Institut National de la Recherche Scientifique [Québec] (INRS)

Subjects
In situ, Materials science, Diffusion, Energy Engineering and Power Technology, chemistry.chemical_element, 02 engineering and technology, Electrolyte, 010402 general chemistry, 01 natural sciences, law.invention, law, Materials Chemistry, Electrochemistry, Chemical Engineering (miscellaneous), [CHIM]Chemical Sciences, Electrical and Electronic Engineering, ComputingMilieux_MISCELLANEOUS, 021001 nanoscience & nanotechnology, Sulfur, Polyelectrolyte, Cathode, 0104 chemical sciences, chemistry, Chemical engineering, Electrode, Tomography, 0210 nano-technology
Abstract

Polyelectrolytes are promising binders for sulfur cathodes of Li/S batteries, with an ability to control the diffusion of polysulfides into the electrolyte, but their impact on the microstructural ...

Published
2020
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45. Disentangling the Degradation Pathways of Highly Defective PtNi/C Nanostructures – An Operando Wide and Small Angle X-ray Scattering Study

Author

Frédéric Maillard, Laetitia Dubau, Isaac Martens, Tristan Asset, Pierre Bordet, Raphaël Chattot, Nathalie Job, Jakub Drnec, Jaysen Nelayah, Cédric Gommes, Electrochimie Interfaciale et Procédés (EIP ), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), European Synchrotron Radiation Facility (ESRF), Matériaux, Rayonnements, Structure (MRS), Institut Néel (NEEL), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Université Paris Diderot - Paris 7 (UPD7), Laboratoire de Génie Chimique (LGC), and Université de Liège

Subjects
Materials science, Nanostructure, 010405 organic chemistry, Scattering, Small-angle X-ray scattering, Energy-dispersive X-ray spectroscopy, Proton exchange membrane fuel cell, Nanoparticle, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, 010402 general chemistry, 01 natural sciences, Catalysis, Synchrotron, 0104 chemical sciences, law.invention, Chemical engineering, law, Scanning transmission electron microscopy, ComputingMilieux_MISCELLANEOUS
Abstract

Hollow bimetallic nanostructures are perfect systems to unravel the aging mechanisms of both Pt-based alloys and highly defective nanostructures used in proton-exchange membrane fuel cell (PEMFC) cathodes, since the mobility of their surface and bulk atoms leads to detectable chemical (i.e., Ni dissolution) and physical (i.e., decrease of the density of structural defects, collapse of the nanostructure, etc.) changes. In this study, we precisely and dynamically monitored these physicochemical changes on porous hollow PtNi/C nanoparticles during an aging procedure composed of 5000 potential cycles with linear ramps between 0.6 and 1.0 or 1.1 V vs RHE by using (i) synchrotron operando wide- and small-angle X-ray scattering (WAXS and SAXS), (ii) scanning transmission electron microscopy (STEM) in combination with X-ray energy dispersive spectroscopy (X-EDS), and (iii) electrochemical measurements. The synchrotron operando WAXS and SAXS results dynamically correlated the structural changes of the hollow NPs a...

Published
2018
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46. High-Energy Li-Ion Cells: Impact of Electrode Ageing on Second Life Viability

Author

Mikael Cugnet, Eddy Coron, Pierre-Xavier Thivel, Sylvie Genies, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
High energy, Materials science, Renewable Energy, Sustainability and the Environment, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Ion, [CHIM.GENI]Chemical Sciences/Chemical engineering, Chemical engineering, Ageing, Electrode, Materials Chemistry, Electrochemistry, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021
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47. Identification of durable and non-durable FeN x sites in Fe–N–C materials for proton exchange membrane fuel cells

Author

Ying Huang, Andrea Di Cicco, Frédéric Maillard, Jingkun Li, James M. Ablett, Iryna V. Zenyuk, Laetitia Dubau, Frédéric Jaouen, Moulay Tahar Sougrati, Kavita Kumar, Plamen Atanassov, Andrea Zitolo, Ismail Can Oğuz, Ivana Matanovic, Goran Dražić, Tzonka Mineva, 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), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Theoretical Division [LANL], Los Alamos National Laboratory (LANL), Center for Micro-Engineered Materials [Albuquerque] (CMEM), The University of New Mexico [Albuquerque], University of California [Irvine] (UCI), University of California, University of Camerino, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), National Institute of Chemistry Ljubljana, ANR-10-LABX-0044,CEMAM,Center of Excellence in Multifunctional Architectured Materials(2010), ANR-16-CE05-0007,CAT2CAT,Des catalyseurs aux cathodes: Une approche d'architecture contrôlée d'électrode pour pile PEM à base de métaux abondants(2016), ANR-10-LABX-0005,CheMISyst,CHEmistry of Molecular and Interfacial Systems(2010), European Project: 779366,CRESCENDO, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), University of California [Irvine] (UC Irvine), University of California (UC), and Università degli Studi di Camerino = University of Camerino (UNICAM)

Subjects
Proton exchange membrane fuel cell, chemistry.chemical_element, Bioengineering, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, Biochemistry, Catalysis, Mössbauer spectroscopy, Moiety, [CHIM]Chemical Sciences, Spectroscopy, Inert gas, chemistry.chemical_classification, Process Chemistry and Technology, Polymer, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Chemical engineering, 0210 nano-technology, Platinum
Abstract

International audience; While Fe-N-C materials are a promising alternative to platinum for catalyzing oxygen reduction in acidic polymer fuel cells, limited understanding of their operando degradation restricts rational approaches towards improved durability. Here we show that Fe-N-C catalysts initially comprising two distinct FeNx sites (S1 and S2) degrade via the transformation of S1 into iron oxides while the structure and number of S2 were unmodified. Structure-activity correlations drawn from end-of-test 57Fe Mössbauer spectroscopy reveal that both sites initially contribute to the ORR activity but only S2 significantly contributes after 50 h of operation. From in situ 57Fe Mössbauer spectroscopy in inert gas coupled to calculations of the Mössbauer signature of FeNx moieties in different electronic states, we identify S1 to be a high-spin FeN4C12 moiety and S2 a low- or intermediate spin FeN4C10 moiety. These insights lay the ground for rational approaches towards Fe-N-C cathodes with improved durability in acidic fuel cells.

Published
2020
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48. Durability of Alternative Metal Oxide Supports for Application at a Proton-Exchange Membrane Fuel Cell Cathode—Comparison of Antimony- and Niobium-Doped Tin Oxide

Author

Annette Mosdale, Frédéric Maillard, Ignacio Jiménez-Morales, Sara Cavaliere, Laetitia Dubau, Renaut Mosdale, Marian Chatenet, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), 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), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Paxitech, and PaxiTech SAS

Subjects
Control and Optimization, Materials science, antimony-doped tin oxide, Oxide, Energy Engineering and Power Technology, Proton exchange membrane fuel cell, 02 engineering and technology, loose tube, 010402 general chemistry, Electrochemistry, 01 natural sciences, lcsh:Technology, Corrosion, law.invention, chemistry.chemical_compound, law, Electrical and Electronic Engineering, Engineering (miscellaneous), metal oxide support, Renewable Energy, Sustainability and the Environment, Tin dioxide, lcsh:T, Membrane electrode assembly, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Tin oxide, degradation mechanism, Cathode, 0104 chemical sciences, chemistry, Chemical engineering, durability, proton-exchange membrane fuel cell, niobium-doped tin oxide, 0210 nano-technology, Energy (miscellaneous)
Abstract

In this study, the resistance to corrosion of niobium-doped tin dioxide (Nb-doped SnO2, NTO) and antimony-doped tin oxide (Sb-doped SnO2, ATO) supports has been probed for proton-exchange membrane fuel cell (PEMFC) application. To achieve this goal, ATO or NTO supports with loose-tube (fiber-in-tube) morphology were synthesized using electrospinning and decorated with platinum (Pt) nanoparticles. These cathode catalysts were submitted to two different electrochemical tests, an accelerated stress test following the EU Harmonised Test Protocols for PEMFC in a single cell configuration and an 850 h test in real air-breathing PEMFC systems. In both cases, the dissolution of the doping element was measured either by inductively coupled plasma mass spectrometry (ICP−MS) performed on the exhaust water or by energy dispersive X-ray spectrometry (X-EDS) analysis on ultramicrotomed membrane electrode assembly (MEA), and correlated to the performance losses upon ageing. It appears that the NTO-based support leads to lower performances than the ATO-based one, mainly owing to the low electronic conductivity of NTO. However, in the case of ATO, dissolution of the Sb doping element is non-negligible and represents a major issue from a stability point-of-view.

Published
2020
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49. High performance direct borohydride fuel cell using bipolar interfaces and noble metal-free Ni-based anodes

Author

Zhongyang Wang, Antoine Bonnefont, Guillaume Braesch, Elena R. Savinova, Marian Chatenet, Alexandr G. Oshchepkov, Vijay Ramani, Shrihari Sankarasubramanian, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), University of Chicago, Washington University in Saint Louis (WUSTL), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Chatenet, Marian, Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), and Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Alkaline fuel cell, Materials science, PGM-free anode, 02 engineering and technology, engineering.material, 010402 general chemistry, Electrocatalyst, 7. Clean energy, 01 natural sciences, law.invention, Sodium borohydride, chemistry.chemical_compound, Direct Borohydride Fuel Cell (DBFC), Coating, law, Direct borohydride fuel cell, General Materials Science, Alkaline Fuel Cell (AFC), Renewable Energy, Sustainability and the Environment, [SPI.NRJ]Engineering Sciences [physics]/Electric power, General Chemistry, 021001 nanoscience & nanotechnology, Hydrogen peroxide, Cathode, Bipolar interface, 0104 chemical sciences, Anode, Borohydride Oxidation Reaction (BOR), chemistry, Chemical engineering, [CHIM.OTHE] Chemical Sciences/Other, engineering, Noble metal, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other, [SPI.NRJ] Engineering Sciences [physics]/Electric power
Abstract

International audience; Due to its unmatched theoretical voltage of 2.18 V, direct alkaline fuel cell using sodium borohydride solution at the anode and hydrogen peroxide at the cathode, represents a promising power source for high energy density applications. However, its development faces several challenges. Here we demonstrate a BH4-/H2O2 direct borohydride fuel cell (DBFC) with a platinum group metal (PGM)-free anode, which delivers unprecedented combination of 2.0 V open-circuit voltage and peak power density of 446 mW cm-2. This exceptionally high cell voltage is enabled by combining a pH-gradient-enabled microscale bipolar interface (PMBI), a Ni anode obtained by electrodeposition of Ni nanoparticles on an electrochemically-etched Ni felt (eNFT), and a specially-designed simple but efficient coating procedure to deposit anion-exchange ionomer on the anode surface. The PMBI efficiently separates the drastically-disparate pH of the anolyte and the catholyte, the NiED/eNFT anode provides high surface area for efficient electrocatalysis and open porosity for fast mass-transport, while the coating procedure allows preserving Ni in metallic state, the latter being prerequisite for high anode performance. This work details how such fully nickel-based anodes are obtained and demonstrates why their BOR activity and stability outperforms that of PGM-based anodes.

Published
2020
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50. Electrochemical hydrogen compression and purification versus competing technologies – Part I: pros and cons

Author

Florence Druart, Marine Trégaro, Maha Rhandi, Marian Chatenet, Jonathan Deseure, Chatenet, Marian, Electrochimie Interfaciale et Procédés (EIP), Laboratoire d'Electrochimie et de Physico-chimie des Matériaux et des Interfaces (LEPMI), Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)

Subjects
Hydrogen, Computer science, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Hydrogen purifier, Electrochemical hydrogen compressor, [CHIM.GENI]Chemical Sciences/Chemical engineering, Process engineering, ComputingMilieux_MISCELLANEOUS, Hydrogen production, business.industry, [CHIM.GENI] Chemical Sciences/Chemical engineering, Scale (chemistry), Fossil fuel, [CHIM.CATA] Chemical Sciences/Catalysis, General Medicine, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Renewable energy, chemistry, 13. Climate action, Electricity, 0210 nano-technology, business
Abstract

It is undisputed that hydrogen will play a great role in our future energetic mix, because it enables the storage of renewable electricity (power-to-H2) and the reversible conversion into electricity in fuel cell, not to speak of its wide use in the (petro)chemical industry. Whereas in these applications, pure hydrogen is required, today's hydrogen production is still largely based on fossil fuels and can therefore not be considered pure. Therefore, purification of hydrogen is mandatory, at a large scale. In addition, hydrogen being the lightest gas, its volumetric energy content is well-below its competing fuels, unless it is compressed at high pressures (typically 70 MPa), making compression unavoidable as well. This contribution will detail the means available today for both purification and for compression of hydrogen. It will show that among the available technologies, the electrochemical hydrogen compressor (EHC), which also enables hydrogen purification, has numerous advantages compared to the classical technologies currently used at the industrial scale. EHC has their thermodynamic and operational advantages, but also their ease of use. However, the deployment of EHCs will be viable only if they reach sufficient performances, which implies some specifications that their base materials should stick to. The present contribution will detail these specifications.

Published
2020

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