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1. Investigation of liquid water heterogeneities in large area PEM fuel cells using a pseudo-3D multiphysics model

Author: Jean-Philippe Poirot-Crouvezier, M. Chandesris, Yann Bultel, Arnaud Morin, F. Courtois, E. Tardy, Département de l'Electricité et de l'Hydrogène pour les Transports (DEHS), 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)-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), Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), 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]), Département Etude des Réacteurs (DER), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), 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), ARC-Nucleart CEA Grenoble (NUCLEART), 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), Bultel, Yann, Electrochimie Interfaciale et Procédés (EIP ), 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: Materials science, [SPI.GPROC] Engineering Sciences [physics]/Chemical and Process Engineering, Multiphysics, Flow (psychology), Proton exchange membrane fuel cell, 02 engineering and technology, 7. Clean energy, 01 natural sciences, 010305 fluids & plasmas, Proton Exchange Membrane Fuel Cell Water transport Two-phase flow Computer simulations Neutron imaging, Stack (abstract data type), 0103 physical sciences, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], Fluid Flow and Transfer Processes, Water transport, Gas diffusion electrode, Mechanical Engineering, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Mechanics, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Durability, Model predictive control, 13. Climate action, 0210 nano-technology, [SPI.NRJ] Engineering Sciences [physics]/Electric power
Abstract: International audience; Effective management of the liquid water and heat produced in Proton Exchange Membrane Fuel Cell (PEMFC) is necessary to increase both its performance and durability. In previous works, a pseudo-3D physic-based model of heat and water transport in fuel cells was developed and has been validated against experimental temperature and current density data. In this study, liquid water measurement obtained from neutron imaging tests is compared with numerical results. The model is able to predict qualitatively the presence of liquid water with a good accuracy taking into account the real Bipolar Plate (BP) design. Based on the reliability of the predictions at this first order in-plane space scale, the model has been used to compute the thickness of liquid water through the plane of the cell, in the different components of the stack, Gas Channel (GC) or Gas Diffusion Electrode (GDE). Our two-phase flow formulation has also been compared to more classical phase-separated two-phase flow model. A good accordance is observed for low saturations. The good agreement between predictions and measurement results supports the capability of our model to be employed in predictive control strategies or to design innovative Bipolar Plate (BP) at lower cost compared to experimental tests.
Published: 2019
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2. 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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3. Direct Evidence of the Role of Co or Pt, Co Single-Atom Promoters on the Performance of MoS2 Nanoclusters for the Hydrogen Evolution Reaction

Author: Luz A. Zavala, Kavita Kumar, Vincent Martin, Frédéric Maillard, Françoise Maugé, Xavier Portier, Laetitia Oliviero, Laetitia Dubau, Laboratoire catalyse et spectrochimie (LCS), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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), Centre de recherche sur les Ions, les MAtériaux et la Photonique (CIMAP - UMR 6252), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Nanomatériaux, Ions et Métamatériaux pour la Photonique (NIMPH), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), and ANR Carnot Energie et Systèmes de Propulsion (ESP)ANR Carnot Energies du futur (EF)
Subjects: Non-noble electrocatalyst, Hydrogen Evolution Reaction (HER), Single Atom Promoted Molybdenum Sulfides, Proton Exchange Membrane Water Electrolyzer (PEMWE), [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Durability, Catalysis
Abstract: International audience; Developing alternatives to platinum (Pt) and iridium (Ir) in proton exchange membrane water electrolyzers is crucial on the way to viable energy provision schemes. However, although it seems difficult to substitute Ir, alternatives exist for Pt at the PEMWE cathode. Here, we report on the synthesis and the characterization of efficient and durable hydrogen evolution reaction (HER) nanocatalysts based on MoS2 supported on high surface area carbon. Citric acid was used as a chelating agent to control the size of the crystallites (1.4 nm) and thus the density of active sites (slab edges). Inspired by successful approaches in catalysis for hydrodesulfurization reactions, conventional 2H MoS2 was sequentially doped with cobalt (Co) then 1 wt. % of Pt. Overpotentials of 188 mV, 140 and 118 mV at 10 mA cm-2 are reported for MoS2/C, Co-MoS2/C and Pt1%-CoMoS2/C, respectively. This result is attributed to the weakening of Hads binding energy of the promoted MoS2 edge active sites (because the promoting atoms are mostly located at the edges). Associated with small metal dissolution rates (monitored in situ, during HER), our findingsdemonstrate that metal promotion (doping) is a promising route to replace platinum by earth-abundant elements in acidic water electrolyzers.
Published: 2023
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4. Imaging the strain evolution of a platinum nanoparticle under electrochemical control

Author: Clément Atlan, Corentin Chatelier, Isaac Martens, Maxime Dupraz, Arnaud Viola, Ni Li, Lu Gao, Steven J. Leake, Tobias U. Schülli, Joël Eymery, Frédéric Maillard, Marie-Ingrid Richard, 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), Nanostructures et Rayons X (NRX), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Eindhoven University of Technology [Eindhoven] (TU/e), and European Project: 818823,CARINE
Subjects: [PHYS.MECA.MEMA]Physics [physics]/Mechanics [physics]/Mechanics of materials [physics.class-ph], Mechanics of Materials, Mechanical Engineering, General Materials Science, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, General Chemistry, Condensed Matter Physics
Abstract: International audience; Surface strain is widely employed in gas phase catalysis and electrocatalysis to control the binding energies of adsorbates on active sites. However, in situ or operando strain measurements are experimentally challenging, especially on nanomaterials. Here, we exploit coherent diffraction at the new 4 th generation Extremely Brilliant Source at the European Synchrotron Radiation Facility (ESRF-EBS) to map and quantify strain inside individual Pt catalyst nanoparticles under electrochemical control. 3D nanoresolution strain microscopy together with density functional theory and atomistic simulations show for the first time evidence of heterogeneous and potential-dependent strain distribution between highly-coordinated ({100} and {111} facets) and under-coordinated atoms (edges and corners) as well as evidence of strain propagation from the surface to the bulk of the nanoparticle. These dynamic structural relationships directly inform the design of strain-engineered nanocatalysts for energy storage and conversion applications.
Published: 2023
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5. In situ and operando 3D imaging of Pt and Pd electrocatalytic nanocrystals

Author: Atlan, Clément, Chatelier, Corentin, Viola, Arnaud, Dupraz, Maxime, Leake, Steven, Eymery, J., Maillard, Frédéric, Richard, Marie‐ingrid, 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), Nanostructures et Rayons X (NRX), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), The Minerals, Metals & Materials Society (TMS), European Project: 818823,CARINE, European Project: 952184,HERMES, and Nanostructures et Rayonnement Synchrotron (NRS )
Subjects: [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: International audience; Structural properties of transition metal are critical to understand the catalytic behavior of electrochemical processes. Here we show that 200 nm Pt and 500 nm Pd nanocrystals can be probed in situ and operando through Bragg Coherent X-ray Diffraction Imaging. This lens-less technique enables determining the morphology as well as mapping the strain and displacement fields of such nanoparticles. By measuring the Pt 002 Bragg reflection we show evidence of heterogeneous and potential-dependent strain distribution between highly-coordinated ({100} and {111} facets) and under-coordinated atoms (edges and corners) as well as evidence of strain propagation from the surface to the bulk of the nanoparticle. This allows to unveil adsorption sites. We also demonstrate that the formation of highly strained palladium hydride nanocrystals can be tracked under potential control. Even though the beta phase (hydrogen rich) Bragg peak comes and vanishes at relevant potentials, the nanocrystal does not recover its pristine morphology.
Published: 2023

6. FeNC Oxygen Reduction Electrocatalyst with High Utilization Penta‐Coordinated Sites

Author: Jesús Barrio, Angus Pedersen, Saurav Ch. Sarma, Alexander Bagger, Mengjun Gong, Silvia Favero, Chang‐Xin Zhao, Ricardo Garcia‐Serres, Alain Y. Li, Qiang Zhang, Frédéric Jaouen, Frédéric Maillard, Anthony Kucernak, Ifan E. L. Stephens, Maria‐Magdalena Titirici, Imperial College London, Department of Chemistry [Imperial College London], Department of Chemical Engineering, Tsinghua University, Physiochimie des Métaux (PMB), 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), Bolin Centre for Climate Research, Stockholm University, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), 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), WPI Advanced Institute for Materials Research (WPI-AIMR), Tohoku University [Sendai], ANR-17-EURE-0003,CBH-EUR-GS,CBH-EUR-GS(2017), ANR-11-LABX-0003,ARCANE,Grenoble, une chimie bio-motivée(2011), European Project: 866402,NitroScission, European Project: 892614,HAEMOGLOBIN, and European Project: 896637 ,DimerCat
Subjects: Mechanics of Materials, Mechanical Engineering, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Atomic Fe in N-doped carbon (FeNC) electrocatalysts for oxygen (O$_2$) reduction at the cathode of proton exchange membrane fuel cells (PEMFCs) are the most promising alternative to platinum-group-metal catalysts. Despite recent progress on atomic FeNC O$_2$ reduction, their controlled synthesis and stability for practical applications remains challenging. A two-step synthesis approach has recently led to significant advances in terms of Fe-loading and mass activity; however, the Fe utilisation remains low owing to the difficulty of building scaffolds with sufficient porosity that electrochemically exposes the active sites. Herein, we addressed this issue by coordinating Fe in a highly porous nitrogen doped carbon support (~3295 m$^2$ g$^{-1}$), prepared by pyrolysis of inexpensive 2,4,6triaminopyrimidine and a Mg$^{2+}$ salt active site template and porogen. Upon Fe coordination, a high electrochemical active site density of 2.54×10$^{19}$ sites g$_{FeNC}$$^{-1}$ and a record 52% FeN$_x$ electrochemical utilisation based on in situ nitrite stripping was achieved. The Fe single atoms are characterised pre-and post-electrochemical accelerated stress testing by aberration-corrected high-angle annular dark field scanning transmission electron microscopy, showing no Fe clustering. Moreover, ex situ X-ray absorption spectroscopy and low-temperature Mössbauer spectroscopy suggest the presence of penta-coordinated Fe sites, which were further studied by density functional theory calculations.
Published: 2023
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7. Breathing Pt nanoparticle imaged using in situ BCDI

Author: Atlan, Clément, Chatelier, Corentin, Martens, Isaac, Dupraz, Maxime, Leake, Steven, Richard, Marie-Ingrid, Viola, Arnaud, Maillard, Frédéric, 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 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), European Synchroton Radiation Facility [Grenoble] (ESRF), ESRF, European Project: 818823,CARINE, and European Project: 952184,HERMES
Subjects: [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; The relationship between surface strain and the rate of a (electro-)catalytic reaction was unveiled by Hammer and Nørskov using density functional theory (DFT) calculations [1,2]. They proposed that the rate of the sluggish oxygen reduction reaction (ORR) would be enhanced on Pt-based catalysts binding *OH species ca. 0.10 - 0.15 eV more weakly than Pt(111), [1, 2] later experimentally verified using a Pt3Ni(111)-skin surface.[3] Nevertheless these predictions did not translate to Pt-based nanocatalysts, in part because these feature present multiple catalytic sites with a range of binding energies. Also, DFT calculations consider catalytic surfaces in vacuum, i.e. in the absence of water molecules and electric field. Hence, an in situ picture of how strain is distributed on Pt-based surfaces is still lacking.In this contribution, we took benefit of recent advances in Bragg Coherent Diffraction Imaging (BCDI) [4, 5] and of the fourth generation Extremely Brilliant Source of the European Synchrotron (ESRF-EBS, Grenoble, France) to map strain over Pt nanoparticles in electrochemical environment. Our results reveal that strain is heterogeneously distributed between highly- and weakly-coordinated surface atoms, and propagates from the surface to the bulk of the Pt nanoparticle as (bi)sulphates anions adsorb on the surface.
Published: 2023

8. From multi-physics to electrical circuit models of aged graphite electrodes of Lithium-ion battery

Author: Oumaima Chaouachi, Marion Chandesris, Jean-Michel Rety, Yann Bultel, Forsee Power, 1 Boulevard Hippolyte Marques, F-75013 Paris, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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 the French National Association of Research and Technology (CIFRE 2017/0705)
Subjects: Renewable Energy, Sustainability and the Environment, [PHYS.MPHY]Physics [physics]/Mathematical Physics [math-ph], Materials Chemistry, Electrochemistry, Condensed Matter Physics, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials
Abstract: International audience; A two-step up-scaling methodology is established to determine a temporal Electric Equivalent Circuit (EEC) model of aged graphite electrodes. The methodology is fed with original experimental results of graphite impedance spectra obtained upon aging on graphite-NMC pouches instrumented with reference electrodes. An analytical expression is first derived which includes the impedance contributions from interfacial kinetics, double-layer adsorption, solid-phase diffusion processes in the graphite particles as well as lithium diffusion through the SEI layer. The derivation of the temporal EEC model from this analytical expression using Foster series allows to link the EEC model parameters to materials properties and to tune the accuracy of the model by choosing the number of RC elements in the series. The validity of the model is ascertained by comparison with the experimental data obtained at different aging time and for two cycling temperature conditions. In particular, accounting for lithium diffusion through the SEI is necessary to capture the evolution of the impedance spectra of significantly aged graphite electrodes.
Published: 2023
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9. Review on the Degradation Mechanisms of Metal-N-C Catalysts for the Oxygen Reduction Reaction in Acid Electrolyte: Current Understanding and Mitigation Approaches

Author: Kumar, Kavita, Dubau, Laetitia, Jaouen, Frédéric, Maillard, Frédéric, 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), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), 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), ANR-21-CE05-0021,DEEP,Pile à combustible à membrane échangeuse d'anions alliant haute performance et chargement en métaux précieux ultrabas(2021), and European Project: 779366,CRESCENDO
Subjects: [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; One bottleneck hampering the widespread use of fuel cell vehicles, in particular of proton exchange membrane fuel cells (PEMFCs), is the high cost of the cathode where the oxygen reduction reaction (ORR) occurs, due to the current need of precious metals to catalyse this reaction. Electrochemists tackle this issue in the short/medium term by developing catalysts with improved utilization or efficiency of platinum, and in the longer term, by developing catalysts based on Earth-abundant elements. Considerable progress has been achieved in the initial performance of Metal-Nitrogen-Carbon (Metal-N-C) catalysts for the ORR, especially with Fe-N-C materials. However, until now, this high performance cannot be maintained for sufficiently long time in operating PEMFC. The identification and mitigation of the degradation mechanisms of Metal-N-C electrocatalysts in the acidic environment of PEMFCs has therefore become an important research topic. Here, we review recent advances in the understanding of the degradation mechanisms of Metal-N-C electrocatalysts, including the recently identified importance of combined oxygen and electrochemical potential. Results obtained in liquid-electrolyte and PEMFC device are discussed, as well as insights gained from in situ and operando techniques. We also review the mitigation approaches that the scientific community has hitherto investigated to overcome the durability issues of Metal-N-C electrocatalysts.
Published: 2023
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10. 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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11. Safety Evaluation of All-Solid-State Batteries: An Innovative Methodology Using In Situ Synchrotron X-ray Radiography

Author: Juliette Charbonnel, Natacha Darmet, Claire Deilhes, Ludovic Broche, Magali Reytier, Pierre-Xavier Thivel, Rémi Vincent, Université Grenoble Alpes, CEA, Liten, DEHT, 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 European Synchroton Radiation Facility [Grenoble] (ESRF)
Subjects: [CHIM.GENI]Chemical Sciences/Chemical engineering, Materials Chemistry, Electrochemistry, Energy Engineering and Power Technology, Chemical Engineering (miscellaneous), Electrical and Electronic Engineering
Abstract: International audience
Published: 2022
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12. Operando potential-induced strain heterogeneity of a breathing Pt nanoparticle: MS40 - Operando and in-situ crystallographic studies

Author: Atlan, Clément, Chatelier, Corentin, Viola, Arnaud, Dupraz, Maxime, Leake, Steven, Eymery, J., Maillard, Frédéric, Richard, Marie‐ingrid, 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), Nanostructures et Rayonnement Synchrotron (NRS ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), and European Project: 818823,CARINE
Subjects: [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Pt nanoparticles and their alloys are frequently used as catalysts in a large number of (electro)chemical processes. Understanding how the structure of these catalysts evolve during the reaction is a major challenge to optimize their catalityc performance and activity. Since coherent X-ray diffraction imaging is a nondestructive technique, it allows for the in situ and operando 3D mapping of the sctuctural response of single nanoparticles during electrochemical reaction (i.e. for diffferent electrode potentials) and for different types of electrolyte. Here, we show that the use of this technique allows to follow the 3D evolution of the strain of a Pt nanoparticle during an electrochemical reaction (see Figure 1). More precisely, we show evidence of heterogeneous and potential-dependent strain distribution between highly-coordinated ({100} and {111} facets) and under coordinated atoms (edges and corners) as well as evidence of strain propagation from the surface to the bulk of the nanoparticle (see Figure 2). The heterogeneity of strain distribution depends on the electrode potential and reaches as large as 0.08 % at oxygen reduction reaction-relevant potential. These results provide dynamic structural insights to better simulate and design efficient nanocatalysts for energy storage and conversion applications.
Published: 2022

13. Imaging the Breathing of a Platinum Nanoparticle in Electrochemical Environment

Author: Atlan, Clément, Chatelier, Corentin, Dupraz, Maxime, Martens, Isaac, Viola, Arnaud, Li, Ni, Gao, Lu, Leake, Steven J., Schülli, Tobias U., Eymery, Joël, Maillard, Frédéric, Richard, Marie-Ingrid, 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), 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), Eindhoven University of Technology [Eindhoven] (TU/e), ANR-19-ENER-0008,BRIDGE,Vers l'intégration de catalyseurs performants dans des électrodes de pile à combustible efficaces(2019), and European Project: 818823,CARINE
Subjects: Condensed Matter - Materials Science, Strain 3D, Coherent diffraction imaging, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Platinum and palladium catalysts, Electrocatalysis in situ and operando, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: Surface strain is widely used in gas phase catalysis and electrocatalysis to control the binding energies of adsorbates on metal surfaces. However, $in$ $situ$ or $operando$ strain measurements are experimentally challenging, especially on nanomaterials. Here, we take advantage of the 4$^{th}$ generation Extremely Brilliant Source at the European Synchrotron Radiation Facility (ESRF-EBS, Grenoble, France) to quantify the distribution of strain inside a Pt nanoparticle, and to determine its morphology in an electrochemical environment. Our results show for the first time evidence of heterogeneous and potential-dependent strain distribution between highly-coordinated ({100} and {111} facets) and under-coordinated atoms (edges and corners) as well as evidence of strain propagation from the surface to the bulk of the nanoparticle. These results provide dynamic structural insights to better simulate and design efficient nanocatalysts for energy storage and conversion applications.
Published: 2022

14. 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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15. Structural disorder in ORR electrocatalysis: operation mode, practical descriptors to quantify and foreseen challenges

Author: Chattot, Raphaël, Atlan, Clément, Viola, Arnaud, Chatelier, Corentin, Martens, Isaac, Roiron, Camille, Drnec, Jakub, Bordet, Pierre, Richard, Marie‐ingrid, Dubau, Laetitia, Maillard, Frédéric, 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 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), European Synchroton Radiation Facility [Grenoble] (ESRF), Matériaux, Rayonnements, Structure (NEEL - MRS), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), ANR-19-ENER-0008,BRIDGE,Vers l'intégration de catalyseurs performants dans des électrodes de pile à combustible efficaces(2019), ANR-14-CE05-0003,HOLLOW,Au-delà des électrocatalyseurs traditionnels : des nanoparticules creuses de métal noble pour applications PEMFC(2014), European Project: 818823,CARINE, Maillard, Frédéric, Vers l'intégration de catalyseurs performants dans des électrodes de pile à combustible efficaces - - BRIDGE2019 - ANR-19-ENER-0008 - ANR-BMBF - VALID, Appel à projets générique - Au-delà des électrocatalyseurs traditionnels : des nanoparticules creuses de métal noble pour applications PEMFC - - HOLLOW2014 - ANR-14-CE05-0003 - Appel à projets générique - VALID, and Coherent diffrAction foR a look Inside Nanostructures towards atomic rEsolution: catalysis and interface - CARINE - 818823 - INCOMING
Subjects: [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract: International audience; Due to strain and ligand effects, the simultaneous presence of concave and convex surfaces and their highly-defective nanostructure (atomic vacancies, grain boundaries), highly defective hollow PtNi/C electrocatalysts have proven to enhance remarkably the oxygen reduction reaction (ORR) kinetics [1,2]. Likewise, PtNi aerogel [3], jagged PtNi nanowires [4,5] feature both high concentration of structural defects and enhanced ORR activity. On the other hand, and inspired from single crystal approach, nanostructured octahedral-shaped PtNi/C electrocatalysts exhibiting only Pt(111) facets are among the most active ORR electrocatalysts [6,7]. This presentation will show how structure-activity-stability relationships of these two classes of materials can be unified via two descriptors derived from structural and electrochemical parameters respectively [8,9]. A special emphasis will be given on the stability trends of these two families of ORR electrocatalysts.
Published: 2022

16. Anode Defects’ Propagation to the Electrolyte and Catalyst Layers in Polymer Electrolyte Membrane Fuel Cells

Author: Touhami Salah, Marie Crouillere, Julia Mainka, Jérôme Dillet, Christine Nayoze-Coynel, Corine Bas, Laetitia Dubau, Assma El Kaddouri, Florence Dubelley, Fabrice Micoud, Marian Chatenet, Yann Bultel, Olivier Lottin, Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Genèse et Usage d'Interfaces Durables pour l'Energie (GUIDE), 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 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), 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), Electrochimie Interfaciale et Procédés (EIP), and CEA LITEN Grenoble
Subjects: [SPI.NRJ]Engineering Sciences [physics]/Electric power, [SPI.MAT]Engineering Sciences [physics]/Materials
Abstract: Defects known to shorten the lifetime of polymer electrolyte membrane fuel cells (PEMFC) can appear on different membrane electrode assembly (MEA) components and under different forms due to manufacturing processes or operational aging of the fuel cell [1, 2]. Defects-propagation in polymer electrolyte membrane fuel cells membrane electrode assemblies (MEA) is investigated via Accelerated Stress Tests (AST) combining load (hence potential) cycling, load-driven humidity cycling, and open-circuit voltage. Customized MEA with lack of anode catalyst layer at two different locations -near the hydrogen inlet or outlet- are fabricated and subjected to the AST. Periodical electrochemical characterizations are performed using a segmented and instrumented cell, enabling to track the cell performance and anode/cathode electrochemical surface area (ECSA) over the test period with a spatial resolution along the gas channels. These observations are completed by post mortem analyses of the MEA. The MEA accelerated degradation is obvious, with multiple impacts on the cell performance and materials. More specifically, the results brought first evidence of defects propagation in terms of membrane thinning and anode ECSA loss: significant membrane thinning is observed for the defective segments, while anode ECSA loss is measured downstream in the direction of the hydrogen flow. The cathode degradation is poorly affected by the presence of the anode defects. In addition, membrane degradation also appears to propagate downstream the channels when the AST is prolonged for a long period of time. Anode and cathode local potential monitoring during the AST reveals the absence of cathode high-potential excursion, in both the segments with/without initial defects. However, oxygen crossover -toward the hydrogen compartment- is probably detected through slight variations in the anode local potential: this lead to the conclusion that the membrane and anode accelerated degradations are seemingly governed by chemical mechanisms like gas crossover rather than electrochemical mechanisms induced by high-potential excursions. Guilminot, E. et al. Membrane and Active Layer Degradation upon PEMFC Steady-State Operation. J. Electrochem. Soc. 154, B1106 (2007). Dubau, L. et al. A review of PEM fuel cell durability: Materials degradation, local heterogeneities of aging and possible mitigation strategies. Wiley Interdiscip. Rev. Energy Environ. 3, 540–560 (2014). Figure 1
Published: 2022
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17. Description of strontium precipitation in highly concentrated nitric acid

Author: Emilie Baudat, Isabelle Billard, Céline Gautier, Service d'études analytiques et de réactivité des surfaces (SEARS), Département de Physico-Chimie (DPC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, 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 d’analyse en soutien aux exploitants (LASE), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Département de Physico-Chimie (DPC)
Subjects: Health, Toxicology and Mutagenesis, Multipurpose-fitting routine, Speciation, Public Health, Environmental and Occupational Health, Concentrated nitric acid, Pollution, Analytical Chemistry, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Phreeqc, Nuclear Energy and Engineering, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Strontium, Radiology, Nuclear Medicine and imaging, [CHIM.RADIO]Chemical Sciences/Radiochemistry, Spectroscopy
Abstract: International audience; The precipitation of strontium in highly concentrated nitric acid is often used in standard radiochemical methods for $^90$ Sr separation. In this work, the description of Sr behavior in such conditions was studied in the point of speciation simulation. Standard speciation method based on Phreeqc software was considered but two problems underlined the limits of this approach to study this process: inappropriate ionic strength correction model (for I>10 M) and the particular dissociation of nitric acid. To overcome these issues, a multipurpose-fitting routine, Minuit, was used to fit chemical model parameters. A polynomial expression was also added to the model in order to take into account nitric acid dissociation. This alternative was proved successful to calculate the Sr precipitate in highly concentrated nitric acid. Comparison was made with the results obtained with Design of Experiment methodology.
Published: 2022
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18. Physicochemical properties evolution of cathodic catalyst layer and cell performance improvement during PEMFC start-up with mitigation strategies

Author: Timothée Drugeot, Fabrice Micoud, Eric Pinton, Jean-Philippe Poirot, Sébastien Rosini, Laure Guetaz, Lucas Poupin, Yann Bultel, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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: [SPI.NRJ]Engineering Sciences [physics]/Electric power, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Proton Exchange Membrane Fuel Cell is a promising technology to power electric vehicle. To mass-market, one of the technological limitations to overcome concerns improvements in durability[1]. Degradation mechanisms during real-life condition in vehicular operation have been reviewed and authors revealed start-up/shut-down (SU/SD) as critical phases [2]. Indeed, the well-identified reverse current decay mechanism occurs during the H2|Air coexistence in anode side and it is recognized to accelerate Platinum catalyst and carbon support degradations within Cathode Catalyst Layer (CCL)[3,4]. Frequent SU/SD results to a progressive evolution of CCL physiochemical properties, and ultimately, cell performance decay. In this work, a novel Accelerated Stress Test (AST) was designed to mimic realistic potential profile at the cathode side during the SU-phase[5]. By comparing to the well-known triangular profile recommended by SU DoE[6], our profile adds a high potential plateau at 1.6 V during 1.5 s relative to the H2|Air front propagation. A 100-cm² single cell with state-of-art flow field and commercial MEA is used. This ageing test is coupled with electrochemical characterization by voltammogram, CO / CO2 gas analysis at the cathode outlet and performance measurement by polarization curve to assess a clear insight into degradation mechanisms. Afterwards a sensitivity study is performed onto both plateau potential value (Efront) and its exposure time (tfront). Results validate that lowering cathodic potential during H2|Air front propagation by dummy load application and lowering its exposure time by accelerating H2 introduction are promising mitigation strategies. In further details, degradation mechanisms within CCL are more sensitive to potential parameter than the exposure time. Pt dissolution and redeposition are revealed predominant at lower potential range (1.0-1.4 V) whereas carbon support corrosion and Pt detachment are at higher potential range (1.4-1.6 V). Otherwise, this work shows also that SU-AST cycling with an Efront value equal to 1.0 and 1.2 V improves cell performance despite a loss of ECSA and carbon support. A beneficial CCL modification at the beginning of test is suspected, which could lead to an enhancement of future break-in protocol assuming optimize carbon support properties and thus cell performance at high current densities.
Published: 2022

19. Coupling experiments and modeling: towards a better understanding of PEMFC operation

Author: Vandenberghe, Florent, Schott, Pascal, Micoud, Fabrice, Morin, Arnaud, Chatenet, Marian, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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: [SPI]Engineering Sciences [physics], [CHIM]Chemical Sciences, [SPI.TRON]Engineering Sciences [physics]/Electronics
Abstract: International audience; Despite many improvements, PEMFC systems still suffer technological limitations, some of which being linked to the materials cost, performance and durability of the cathode catalyst layer. Combining experiments and modeling enables to characterize and better understand the behaviour of the carbon-supported platinum (Pt/C) electrocatalyst, its utilization/effectiveness in PEMFC cathode catalyst layers and to be able to predict the performance and durability of PEMFC. In this work, physico-chemical and electrochemical measurements are performed from the scale of the raw Pt/C materials up to the complete catalyst layer, to gather as much information as possible on the catalytic layer micro-structure and its operating properties. During experimental performance measurements in PEMFC differential-single cell (1.8 cm² under high reactant stoichiometry), reversible performance gains/losses can be observed. This behaviour is often ascribed to variable hydration state of the ionomer in the catalyst layer and the bulk membrane and also to the evolution of platinum surface states due to oxides partial formation/reduction. In parallel; several models have been developed to simulate one or combined mechanisms leading to the performance1 and degradation of cell components. Based on our experimental work and data sets, the behaviour of the Pt/C electrocatalysts has been studied in order to introduce new electrocatalytic features in one-dimensional models, especially the Pt surface oxide formation and reduction through basic reactions linked to the surface state of Pt as well as to bulk Pt oxide formation via chemical place exchange reaction. This preliminary step was successfully implemented into a complete performance model for the O$_2$ reduction reaction at the cathode, that better describes the physical and electrochemical phenomena involved in very low loaded cathode catalyst layers during fuel cell operation. Hydration variation of the cathode catalyst layer and Pt oxide formation/reduction are now well described in the model during performance simulation leading to hysteresis phenomena as observed experimentally. Impact of the cathode catalyst layer structure, composition and loading as well as transport properties influence the hysteresis phenomenon and will be discussed.
Published: 2022

20. Dégradation de la membrane perfluorée renforcée en présence d'un défaut de la couche anodique dans une pile à combustible PEMFC

Author: Corine Bas, Marie Crouillere, Florence Dubelley, Marian Chatenet, Laetitia Dubau, Bultel, Y., Sahal Touhami, Olivier Lottin, Assma El Kaddouri, Julia Mainka, Jérôme Dillet, Olivier Chadebec, Cauffet, G., Nayoze-Coynel, C., Micoud, F., Sébastien Rosini, Genèse et Usage d'Interfaces Durables pour l'Energie (GUIDE), 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), Electrochimie Interfaciale et Procédés (EIP), Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Génie Electrique de Grenoble (G2ELab ), 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), and ANR-17-CE05-0003,LOCALI,Dévoiler les mécanismes de propagation des défauts locaux dans les PEMFC, par mesure et exploitation de la distribution de densité de courant locale(2017)
Subjects: [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience
Published: 2022

21. Optimisation de la répartition d eau, de température et de courant dans les piles à combustible de type PEM

Author: Cornet, Marine, Bultel, Yann, Morin, Arnaud, Poirot, Jean-Philippe, Schott, Pascal, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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: [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering
Abstract: International audience
Published: 2022

22. Mapping Strain in Platinum Nanoparticles via Bragg Coherent Diffraction Imaging

Author: Atlan, Clément, Richard, Marie‐ingrid, Martens, Isaac, Dupraz, Maxime, Chatelier, Corentin, Viola, Arnaud, Leake, Steven, Maillard, Frédéric, 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), 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), European Synchroton Radiation Facility [Grenoble] (ESRF), Electrochimie Interfaciale et Procédés (EIP), 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 ), The Electrochemical Society, ANR-19-ENER-0008,BRIDGE,Vers l'intégration de catalyseurs performants dans des électrodes de pile à combustible efficaces(2019), and European Project: 818823,CARINE
Subjects: [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Variations in the interatomic distances lead to altered d-band centre for a given metal, and provide an elegant way to control its activity towards (electro)catalytic reactions (“strain-engineering” approach). The effect of strain was rationalized within the frame of the d-band theory of Hammer and Nørskov in the late 1990s [1,2]. The authors predicted that the rate of the sluggish oxygen reduction reaction (ORR) can be enhanced on catalysts binding *OH ca. 0.10 - 0.15 eV more weakly than Pt(111), [1, 2] and this prediction was experimentally verified using a Pt3Ni(111)-skin surface.[3] Nevertheless, these predictions hardly translated to nanomaterials, because of the wide variety of catalytic sites configurations. Also, the d-band theory mostly considers catalytic surfaces in vacuum, without any effect related to the electrical double layer and adsorption/desorption processes. Hence, an in situ picture of how strain develops on Pt-based surfaces is still lacking.In this contribution, we took benefit of recent advances in Bragg Coherent Diffraction Imaging (BCDI) [4, 5] and of the fourth generation Extremely Brilliant Source of the European Synchrotron (ESRF-EBS, Grenoble, France) to map strain over Pt nanoparticles in situ. Our results show that adsorption of anions causes appearance of compressive strain at under-coordinated (edges and corners) atoms and tensile strain at highly-coordinated ({001} and {111} facets) atoms. Strain heterogeneity increases with the electrode potential and reaches as large as 0.08 %. at ORR-relevant potential. These results provide direct insights into the dynamics of Pt nanoparticles in an electrochemical environment, andhave direct consequences for electrocatalysis in general, and for ORR electrocatalysis in particular.
Published: 2022
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23. Ultrasound interrogation, an operando technique for the monitoring of battery materials

Author: Guillet, Nicolas, Gau, Vincent, Thivel, Pierre-Xavier, Département des Technologies Solaires (DTS), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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), ANR-10-IEED-0014,INES2S,INES2S(2010), CEA, Contributeur MAP, and INES2S - - INES2S2010 - ANR-10-IEED-0014 - IEED - VALID
Subjects: [SPI.NRJ]Engineering Sciences [physics]/Electric power, [PHYS.MECA.ACOU] Physics [physics]/Mechanics [physics]/Acoustics [physics.class-ph], [SPI.NRJ] Engineering Sciences [physics]/Electric power, [PHYS.MECA.ACOU]Physics [physics]/Mechanics [physics]/Acoustics [physics.class-ph]
Abstract: présentation orale (20 min) de quelques résultats de la thèse de Vincent Gau; International audience
Published: 2022

24. 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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25. 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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26. 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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27. 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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28. Electrochemical hydrogen compression and purification versus competing technologies: Part II. Challenges in electrocatalysis

Author: Maha Rhandi, Florence Druart, Marine Trégaro, Marian Chatenet, Jonathan Deseure, 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 Chatenet, Marian
Subjects: Energy carrier, Materials science, Hydrogen, business.industry, 020209 energy, [CHIM.CATA] Chemical Sciences/Catalysis, chemistry.chemical_element, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Medicine, Hydrogen cycle, 021001 nanoscience & nanotechnology, Electrocatalyst, Electrochemistry, 7. Clean energy, Hydrogen purifier, Anode, Catalysis, chemistry, 13. Climate action, 0202 electrical engineering, electronic engineering, information engineering, 0210 nano-technology, Process engineering, business, ComputingMilieux_MISCELLANEOUS
Abstract: Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil feedstock (and to a minor extent from biomass); in consequence the present hydrogen gas on the market is containing non-negligible amounts of impurities that prevent its immediate usage in specialty chemistry or as an energy carrier in fuel cells, e.g. in transportation applications (cars, buses, trains, boats, etc.) that gradually spread on the planet. For these purposes, hydrogen must be of sufficient purity but also sufficiently compressed (at high pressures, typically 70 MPa), rendering purification and compression steps unavoidable in the hydrogen cycle. As shown in the first part of this contribution “Electrochemical hydrogen compression and purification versus competing technologies: Part I. pros and cons”, electrochemical hydrogen compressors (EHCs), which enable both hydrogen purification and compression, exhibit many theoretical (thermodynamic) and practical (kinetics) advantages over their mechanical counterparts. However, in order to be competitive, EHCs must operate in very intensive conditions (high current density and low cell voltage) that can only be reached if their core materials, e.g. the membrane and the electrodes/electrocatalysts, are optimized. This contribution will particularly focus on the properties electrocatalysts must exhibit to be used in EHCs: they shall promote (very) fast hydrogen oxidation reaction (HOR) in presence of impurities, which implies that they are (very) tolerant to poisons as well. This consists of a prerequisite for the operation of the anode of an EHC used for the purification-compression of hydrogen, and the materials developed for poison-tolerance in the vast literature on low-temperature fuel cells, may not always satisfy these two criteria, as this contribution will review.
Published: 2020
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29. 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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30. 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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31. 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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32. Modelling of the anion exchange membrane based water electrolysis

Author: Panda, Ronit-Kumar, Serre, Guillaume, Schott, Pascal, Bultel, Yann, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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: [SPI.NRJ]Engineering Sciences [physics]/Electric power, [INFO.INFO-MO]Computer Science [cs]/Modeling and Simulation
Abstract: International audience; Anion exchange membrane (AEM) electrolysis is the method of hydrogen generation with an Anion Exchange Membrane, using electricity. One of the major advantages of AEM water electrolysis is the replacement of conventional noble metal electrocatalysts with low-cost transition metal catalysts. This device have been modelled in the code MePHYSTO-WE developed by CEA LITEN for the simulation of the electrolyzer performances. The model structure is based on the Bond Graph theory, in which each transport block is represented by a resistive element and each balance block is represented by a capacitive element. The developed multiphysics model for this device also incorporates the transport of liquid water and gaseous products through the porous layers.The equations were solved in MATLAB/ SIMULINK. Finally, the sensitivity analysis incorporates an evaluation and optimisation of the model geometry, operating temperature, concentration of the electrolyte fed into the device and internal characteristics such as porosity and tortuousity of the electrodes and membrane thickness. The main advantage of the model is the assessment of the phenomenon resulting in performance loss of the device , investigating the pH gradient and role of electrolyte concentration on operation as well as understanding the Schroeder paradox for its role on membrane water transport and assessing the key parameters to achieve the desired electrolyser performance. In terms of fabrication of components we also assess the role of membrane and catalyst size and the impact of ionomer content in the membrane and catalysts on the performance.
Published: 2022

33. Modeling of platinum oxides formation and re-duction: a performance model for O2 reduction reaction

Author: Schott, Pascal, Micoud, Fabrice, Morin, Arnaud, Chatenet, Marian, Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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 CEA, Contributeur MAP
Subjects: Hysteresis phenomenon, [SPI.OTHER]Engineering Sciences [physics]/Other, [SPI.OTHER] Engineering Sciences [physics]/Other, Performance model, Reversible degradation, Fuel cell, Modeling
Abstract: International audience; Despite many improvements, PEMFC systems still suffer technological limitations, such as their initial cost and overall durability in real life operation, which prevents widespread industrial deployment. Some of these limitations can be overcome by combining experiments and modeling to characterize and better understand the behaviour of the carbon-supported platinum (Pt/C) electrocatalyst, its utiliza-tion/effectiveness in PEMFC catalyst layers and to be able to predict the performance and durability of PEMFC. This should help making the most relevant choices to accelerate the development processes of PEMFC.In this work, physico-chemical and electrochemical measurements are performed from the scale of the raw Pt/C materials up to the complete catalyst layer, to gather as much information as possible on the catalytic layer micro-structure and its operating properties. Coupling experiments in classic RDE and in PEMFC differential-single cell (1.8 cm² under high reactant stoichiometry) enables to fully characterize the electrochemical properties and behaviour of our materials. During experimental performance meas-urements, reversible performance gains/losses can be observed. This behaviour is often ascribed to variable hydration state of the ionomer in the catalyst layer and the bulk membrane and also to the evolution of platinum surface states due to oxides partial formation/reduction.In parallel; several models have been developed to simulate one or combined mechanisms leading to the performance1 and degradation of cell components2,3. Based on our experimental work and data sets, the behaviour of the Pt/C electrocatalysts has been studied in order to introduce new electrocata-lytic features and especially the Pt surface oxide formation and reduction which is linked to Pt surface state as well as Pt bulk oxide formation via chemical place exchange reaction. This preliminary step was then further developed into a complete performance model for the O2 reduction reaction at the cathode to better describe the physical and electrochemical phenomenon involved in catalyst layers during fuel cell operation. With this new description, the position of the main adsorption/desorption peaks monitored by CV under inert atmosphere and the hysteresis phenomenon on the polarization plot during real fuel cell operation are well captured by the simulation compared to experiment keeping complete physical meaning.
Published: 2022

34. Open data model parameterization of a second-life Li-ion battery

Author: Delphine Riu, Pedro V. H. Seger, Mikael Cugnet, Pierre-Xavier Thivel, Sylvie Genies, Eddy Coron, G2Elab-SYstèmes et Réseaux ELectriques (G2Elab-SYREL), Laboratoire de Génie Electrique de Grenoble (G2ELab ), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Département de l'électricité et de l'hydrogène dans les transports (DEHT), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), 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 ), 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), 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), 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)
Subjects: Battery (electricity), Work (thermodynamics), Renewable Energy, Sustainability and the Environment, Computer science, State of health, 020209 energy, 020208 electrical & electronic engineering, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Energy Engineering and Power Technology, Model parameters, 02 engineering and technology, Span (engineering), Ion, Computational science, Open data, State of charge, [CHIM.GENI]Chemical Sciences/Chemical engineering, 0202 electrical engineering, electronic engineering, information engineering, Electrical and Electronic Engineering, ComputingMilieux_MISCELLANEOUS
Abstract: With the fast expansion of Electric and Hybrid Vehicles, the demand of Li-ion batteries is increasing exponentially. This creates an opportunity for a second life of these cells once they are no longer suitable for their original application. An accurate modelling of the second life can be a powerful tool for these new applications. In this work, we propose a complete second life model parameterization for a Li-Ion cell, with its parameters based on experimental data of NMC/LMO cells cycled through their first and second lives. The resulting model parameters span a State of Health from 80 % to 50 % of the cell original capacity, a State of Charge from 0 to 100 %, two current values and two first life temperature points. The model parameters are presented in an open data fashion in the form of look-up tables, ready to be implemented in simulation softwares.
Published: 2022
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35. Anode defects' propagation in Polymer Electrolyte Membrane Fuel Cells

Author: Salah Touhami, Marie Crouillere, Julia Mainka, Jérôme Dillet, Christine Nayoze-Coynel, Corine Bas, Laetitia Dubau, Assma El Kaddouri, Florence Dubelley, Fabrice Micoud, Marian Chatenet, Yann Bultel, Olivier Lottin, Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Genèse et Usage d'Interfaces Durables pour l'Energie (GUIDE), 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 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), 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), Electrochimie Interfaciale et Procédés (EIP), French Environmental and Energy Management Agency (ADEME), ANR-17-CE05-0016,ECPOR,Couplage Elastocalorique dans les Polymères pour la génération solide du froid(2017), 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: Renewable Energy, Sustainability and the Environment, [SPI.FLUID]Engineering Sciences [physics]/Reactive fluid environment, 05 social sciences, Energy Engineering and Power Technology, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, [CHIM.POLY]Chemical Sciences/Polymers, [CHIM.GENI]Chemical Sciences/Chemical engineering, 0502 economics and business, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, 050207 economics, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, 0210 nano-technology, [CHIM.OTHE]Chemical Sciences/Other
Abstract: International audience; Defects-propagation in polymer electrolyte membrane fuel cells membrane electrode assemblies (MEA) is investigated via Accelerated Stress Tests (AST) combining load (hence potential) and load-driven humidity cycling, and open-circuit voltage. Customized MEA with lack of anode catalyst layer at two different locations -near the hydrogen inlet or outlet- are fabricated and subjected to the AST. Periodical electrochemical characterizations are performed using a segmented cell, enabling to track the cell performance and anode/cathode electrochemical surface area (ECSA) over the test period with a spatial resolution along the gas channels. These observations are completed by post mortem analyses of the MEA.The MEA accelerated degradation is obvious, with multiple impacts on the cell performance and materials. More specifically, the results brought first evidence of defects propagation, in term of anode ECSA loss, in the direction of the hydrogen flow. The cathode ECSA is also impacted, although seemingly homogeneously. Significant membrane thinning is observed for the defective segments, without propagation to the adjacent ones. Anode and cathode local potential monitoring during the AST reveals the absence of cathode high-potential excursion, in both the segments with/without initial defects: the membrane and anode accelerated degradation is governed by chemical mechanisms like gas crossover rather than electrochemical mechanisms induced by high-potential excursions.
Published: 2022
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36. 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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37. Investigation of liquid water heterogeneities in large area PEM fuel cells using a two-phase flow multiphysics model

Author: Tardy, Erwan, Poirot, Jean-Philippe, Schott, Pascal, Morel, Christophe, Serre, Guillaume, Bultel, Yann, Département de l'électricité et de l'hydrogène dans les transports (DEHT), 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)-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), PHELMA Grenoble/Institut Polytechnique, CEA, Contributeur MAP, 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), 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: [PHYS.MECA.THER] Physics [physics]/Mechanics [physics]/Thermics [physics.class-ph], [SPI.NRJ]Engineering Sciences [physics]/Electric power, [PHYS.MECA.THER]Physics [physics]/Mechanics [physics]/Thermics [physics.class-ph], [PHYS.MECA.MEFL] Physics [physics]/Mechanics [physics]/Fluid mechanics [physics.class-ph], [INFO.INFO-MO] Computer Science [cs]/Modeling and Simulation, [PHYS.MECA.MEFL]Physics [physics]/Mechanics [physics]/Fluid mechanics [physics.class-ph], [INFO.INFO-MO]Computer Science [cs]/Modeling and Simulation, [SPI.NRJ] Engineering Sciences [physics]/Electric power
Abstract: International audience; The Proton Exchange Membrane Fuel Cell (PEMFC) is a promising candidate for many applications particular-ly for the transportation in order to decarbonize this sector. Of the barriers, cost and durability represent two of the most significant challenges to achieving clean, reliable and cost-effective fuel cell systems. Proper management of the liquid water and heat produced in PEM fuel cells remains crucial to increase both its performance and durability. Indeed, large liquid water and temperature variations in the cell may accelerate long-term structural problems until irreversible degradation such as membrane micro-cracks (see ref.). A two-phase flow model of a large surface PEM fuel cell is developed with the commercial COMSOL Mul-tiphysics® software using the Finite Element Method (FEM). The model considers the cell as a multilayered system where each layer is accurately in-plane discretized to allow the simulation of local thermodynamics heterogeneities with a reasonable computing time. The numerical results are compared to experimental liquid water measurement obtained from neutron imaging tests in several operating conditions. According to the good agreement, the model is used to predict the distributions of current density, species concentra-tions, water content, etc. in all the components of the cell, while taking into account the real flow-field de-signs. Figure 1 shows the liquid water thickness (a) and the saturation (b) for a dedicated 3 cells stack exper-imentally tested for a high power automotive (Table 1). It appears that the liquid water accumulates at the anode Gas Diffusion Electrode (GDE) on the edges (dark red zone in Figure 1), inducing higher local current density and higher liquid water saturation in the external cathode channels, due to no-proper water convec-tion by hydrogen gas (no anode channel in front of these zones).
Published: 2021

38. Study of la(III) and Ce(III) extraction from aqueous solutions with thermomorphic ionic liquid and betaine extractant

Author: Billard, Isabelle, Papadopoulou, Styliani, Rollet, Anne-Laure, Mériguet, Guillaume, Sirieix-Plénet, Juliette, Cousin, Clément, 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), PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'Electrochimie Physique et Analytique (LEPA), Ecole Polytechnique Fédérale de Lausanne (EPFL), Institut de l'Ouest : Droit et Europe (IODE), Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021

39. Impact d'un vieillissement mécano-chimique ex-situ sur les membranes PFSA pour pile à combustible

Author: Robert, Mylène, El Kaddouri, Assma, Crouillere, Marie, Perrin, Jean-Christophe, Dubau, Laetitia, Dubelley, Florence, Mozet, Kevin, Daoudi, Meriem, Dillet, Jérôme, Morel, Jean-Yves, Leclerc, Sebastien, Bas, Corine, Lottin, Olivier, Genèse et Usage d'Interfaces Durables pour l'Energie (GUIDE), 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), Electrochimie Interfaciale et Procédés (EIP), Laboratoire Énergies et Mécanique Théorique et Appliquée (LEMTA ), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), and Lottin, Olivier
Subjects: [CHIM.POLY] Chemical Sciences/Polymers, [CHIM.POLY]Chemical Sciences/Polymers, [CHIM.GENI]Chemical Sciences/Chemical engineering, [SPI.GPROC] Engineering Sciences [physics]/Chemical and Process Engineering, [CHIM.OTHE] Chemical Sciences/Other, [CHIM.GENI] Chemical Sciences/Chemical engineering, [SPI.FLUID]Engineering Sciences [physics]/Reactive fluid environment, [CHIM.CATA] Chemical Sciences/Catalysis, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, [SPI.FLUID] Engineering Sciences [physics]/Reactive fluid environment, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.OTHE]Chemical Sciences/Other, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021

40. Hot Deformation Behavior of a Beta Metastable TMZF Alloy: Microstructural and Constitutive Phenomenological Analysis

Author: Alberto Moreira Jorge, Claudemiro Bolfarini, Virginie Roche, Ana Paula de Bribean Guerra, 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, constitutive analysis, Thermodynamics, 02 engineering and technology, Flow stress, beta metastable, dynamic recovering, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, Stress (mechanics), Condensed Matter::Materials Science, Hot working, 0103 physical sciences, TMZF, General Materials Science, 010302 applied physics, Mining engineering. Metallurgy, Metals and Alloys, TN1-997, Strain rate, 021001 nanoscience & nanotechnology, spinodal decomposition, Deformation mechanism, Dynamic recrystallization, Hardening (metallurgy), Deformation (engineering), 0210 nano-technology, mechanical twinning
Abstract: A metastable beta TMZF alloy was tested by isothermal compression under different conditions of deformation temperature (923 to 1173 K), strain rate (0.172, 1.72, and 17.2 s−1), and a constant strain of 0.8. Stress–strain curves, constitutive constants calculations, and microstructural analysis were performed to understand the alloy’s hot working behavior in regards to the softening and hardening mechanisms operating during deformation. The primary softening mechanism was dynamic recovery, promoting dynamic recrystallization delay during deformation at higher temperatures and low strain rates. Mechanical twinning was an essential deformation mechanism of this alloy, being observed on a nanometric scale. Spinodal decomposition evidence was found to occur during hot deformation. Different models of phenomenological constitutive equations were tested to verify the effectiveness of flow stress prediction. The stress exponent n, derived from the strain-compensated Arrhenius-type constitutive model, presented values that point to the occurrence of internal stress at the beginning of the deformation, related to complex interactions of dislocations and dispersed phases.
Published: 2021
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41. Anisotropic ionic transport properties in solid PEO based electrolytes

Author: Roselyne Jeanne-Brou, Jonathan Deseure, Trang N.T. Phan, Renaud Bouchet, Didier Devaux, 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), Electrochimie Interfaciale et Procédés (EIP), Institut de Chimie Radicalaire (ICR), and Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: General Chemical Engineering, Electrochemistry, [CHIM]Chemical Sciences
Abstract: International audience
Published: 2022
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42. Matériaux critiques : de leur (mes)usage à leur recyclage

Author: Billard, Isabelle, 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 Billard, Isabelle
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: National audience
Published: 2021

43. Tailoring the metallic and oxide sites of Pd/C and Ni/C catalyst for optimum Hydrogen Oxidation Reaction (HOR) and durability in alkaline media

Author: Ricardo Sgarbi, Marian Chatenet, Huong Doan, 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 Chatenet, Marian
Subjects: Hydrogen oxidation reaction, [CHIM.MATE] Chemical Sciences/Material chemistry, Materials science, Oxide, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, Durability, Catalysis, Metal, chemistry.chemical_compound, Chemical engineering, chemistry, visual_art, visual_art.visual_art_medium, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021

44. Dual-layer catalyst layers for increased proton exchange membrane fuel cell performance

Author: Marian Chatenet, Laetitia Dubau, Yannick Garsany, Rachel Martin, Benjamin D. Gould, Robert W. Atkinson, Karen E. Swider-Lyons, Excet Incorporation, U.S. Naval Research Laboratory, U.S. Naval Research Laboratory, Washington, D. C., Consortium des Moyens Technologiques Communs (CMTC), Institut National Polytechnique de Grenoble (INPG), 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, Energy Engineering and Power Technology, Proton exchange membrane fuel cell, chemistry.chemical_element, 02 engineering and technology, Electrolyte, 7. Clean energy, law.invention, Catalysis, law, 0502 economics and business, Gaseous diffusion, 050207 economics, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, Renewable Energy, Sustainability and the Environment, 05 social sciences, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Cathode, Dielectric spectroscopy, chemistry, Chemical engineering, 0210 nano-technology, Platinum, Carbon
Abstract: International audience; The use of a dual-layer cathode catalyst layer improves the performance of proton exchange membrane fuel cells. To generate single and dual-layer catalyst layers between the gas diffusion media and proton exchange membrane electrolyte, two commercial carbon-supported platinum catalysts with either a high microporosity carbon (Ketjen Black EC-300J) or a low porosity carbon (XC-72 Vulcan carbon) are utilized. We discovered that dual-layer cathode catalyst layers boost maximum power of fuel cells regardless of carbon porosity directionality, with either high surface area carbon at the proton exchange membrane electrolyte or gas diffusion media interface. At 25% relative humidity, a condition that generally inhibits fuel cell performance, a 20% performance boost is realized when using dual-layer cathode CLs. The electrochemical impedance spectroscopy results indicate that cathodes with dual-layer catalyst layer aid in water management due to lower kinetic activity losses of the Pt and improved hydration of the proton exchange membrane electrolyte.
Published: 2021
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45. Modelling and robust control of a second life battery energy storage system

Author: Pedro V. H. Seger, Eddy Coron, Delphine Riu, Pierre-Xavier Thivel, Sylvie Genies, Laboratoire de Génie Electrique de Grenoble (G2ELab ), 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), G2Elab-SYstèmes et Réseaux ELectriques (G2Elab-SYREL), 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 ), 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), 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 ), Département des Technologies Solaires (DTS), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), and ANR-15-IDEX-0002,UGA,IDEX UGA(2015)
Subjects: Battery (electricity), Work (thermodynamics), Control theory, Computer science, [SPI.NRJ]Engineering Sciences [physics]/Electric power, Parameterized complexity, Robust control, Internal resistance, Battery pack, Automotive engineering, Data modeling
Abstract: International audience; With the growth of Electric and Hybrid Vehicles deployment, there is an increasing interest in the development of applications for the second life of their on-board li-ion batteries. However, modeling the ageing of these devices poses new problems, as the uncertainty around their parameters - such as the internal resistance. In this work, we propose to study the impact this ageing has on the operation of a circuit composed of a battery, filters, a DC/DC converter and a charge. For this purpose, an equivalent-circuit non-linear battery model is parameterized with experimental ageing data, so that the behaviour of a Second Life Battery Energy Storage System (SLBESS) can be accurately simulated. A robust H∞ controller is then developed, and we study its performance throughout the entire second life of our battery pack. The obtained results indicate that the controller performances are guaranteed for several operating conditions of the battery, showing that a robust control can successfully compensate the ageing impact.
Published: 2021
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46. 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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47. 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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48. Influence of chromium concentration and partial crystallization on the corrosion resistance of FeCrNiB amorphous alloys

Author: Berger, J.E., Jorge Jr., A.M., Asato, G.H., Roche, V., Jorge, A.M., Koga, G.Y., Kiminami, C.S., Bolfarini, C., Botta, W.J., 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, chemistry.chemical_element, Salt (chemistry), 02 engineering and technology, Electrochemistry, law.invention, Corrosion, Chromium, Differential scanning calorimetry, law, [CHIM]Chemical Sciences, General Materials Science, Crystallization, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Amorphous metal, 020502 materials, Mechanical Engineering, technology, industry, and agriculture, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0205 materials engineering, chemistry, Chemical engineering, Mechanics of Materials, Transmission electron microscopy, 0210 nano-technology
Abstract: The influence of chromium concentration and partial crystallization on the corrosion resistance of the FeCrNiB amorphous alloys was investigated. The samples were produced by melt-spinning equipment. Vacuum heat treatments were used for partial and total crystallization. The study methods used were: X-ray diffraction, differential scanning calorimetry, transmission electron microscopy, and electrochemical tests in high salt concentration media. The results revealed that the concentration of chromium in FeCrNiB amorphous alloys could be reduced significantly, still providing passive film stability. They also show that partial crystallization of FeCrNiB alloys may not be deleterious to the corrosion properties, opening important possibilities for the development of high-performance coatings.
Published: 2021
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49. Optimization of Transports in a Proton-Exchange Membrane Fuel Cell Cathode Catalyst Layer at High Current Densities: A Coupled Modeling/Imaging Approach

Author: Laure Guetaz, Mathias Gerard, M. Barreiros Salvado, Pascal Schott, Yann Bultel, 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 ), and Université Grenoble Alpes (UGA)
Subjects: Materials science, Renewable Energy, Sustainability and the Environment, Proton exchange membrane fuel cell, Condensed Matter Physics, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Cathode catalyst, Chemical engineering, Agglomerate, Materials Chemistry, Electrochemistry, [CHIM]Chemical Sciences, High current, Layer (electronics), ComputingMilieux_MISCELLANEOUS
Abstract: For PEMFC to attain sustainable commercialization, the amount of platinum (catalyst used in conventional PEMFCs) must be significantly reduced, while the performance must be improved. At high current densities, it is found that the nature of the losses is mainly mass transport related [1]. Since the catalyst layer is a highly heterogeneous composite material, understanding its structure is major in order to proceed with the optimization [2]. Therefore, in this work, an approach coupling both numerical modeling and electron microscopy characterization is adopted. An agglomerate/pore-scale model is developed and coupled with a MEA-scale model [3]. The model includes a description of the ionic and gas transport, plus the oxygen reduction reaction under a classical Butler-Volmer formulation. Multiple agglomerate structures are reproduced on the basis of a multiscale characterization setup. From 2-nm isotropic resolution FIB-SEM images, the carbon phase arrangement is built, while from HAADF-STEM a representative platinum particle size histogram is extracted and the particles are distributed on the surface of the carbon particles accordingly. On the HRTEM images, it is possible to observe the Nafion thin film covering the Pt/C agglomerates, and therefore, an average layer thickness can be extracted from these. The local pore size distribution is then obtained using the method of maximum sphere inscription [4], which allows to then determine the local gas diffusivities through the computation of local Knudsen diffusion coefficients. The agglomerate scale structures are upscaled to the catalyst layer scale through a mirroring procedure along the catalyst layer thickness, allowing therefore to analyze the cathode catalyst layer performance for different structure arrangements. In this work, the influence of the operating conditions and of certain structural aspects is analyzed: namely the Pt particle size, carbon aggregate size and Nafion layer thickness. It is found that decreasing the Pt particle size leads to a performance improvement since it is expected that more surface is available for the electrochemical reactions to take place. Still, the improvement margin is dependent on the Pt particle spatial distribution since particles located in zones having large Nafion agglomerates and low Nafion/pore contact simultaneously are found to severely underperform when comparing to particles located in other regions. Increasing the carbon aggregate size is found to be highly detrimental for the overall performance, even though an improved electrical contact is ensured. Such performance decay is linked to the large oxygen concentration drop that arises mainly from the porosity reduction, and to a certain extent, from the mean pore size reduction and the pore tortuosity increase. The Nafion layer thickness parametrization requires a more complex analysis since there is a delicate trade-off that must be explored in the sense that it is highly structure-dependent. On the one hand, an improvement in the ionic conductivity is expected upon increasing the Nafion layer thickness, though on the other hand, an increased resistance to oxygen diffusion is also expected. This trade-off is explored and discussed along with the introduction of the Nafion swelling effect, which is surprisingly not explored in the literature, neither on agglomerate/pore-scale models, nor macroscale models. It is found that increasing the Nafion layer thickness is detrimental for performance only when the porosity is not high enough. To complement the analysis, 'close-to-ideal' structures are built while holding the composition of the reference structures (i.e. electron microscopy based structures). It is found that these idealized structures lead to large performance improvements, showing that there is still much ground for further improvements on the PEMFC cathode catalyst layer. References: [1] J. Benziger, E. Kimball, R. Mejia-Ariza, and I. Kevrekidis. Oxygen mass transport limitations at the cathode of polymer electrolyte membrane fuel cells. AIChE, 57(9):2505-2517, 2010. [2] M.B. Sassin, Y. Garsany, R.W. Atkinson III, R.M.E. Hjelm, and K.E. Swider-Lyons. Understanding the interplay between cathode catalyst layer porosity and thickness on transport limitations en route to high-performance pemfcs. Int. J. Hydrogen Energy, 44(31):16944-16955, 2019. [3] B. Randrianarizafy, P. Schott, M. Chandesris, M. Gerard, and Y. Bultel. Design optimization of rib/channel patterns in a pemfc through performance heterogeneities modelling. Int. J. Hydrogen Energy, 43(18):8907-8926, 2018. [4] V. Novak, F. Stepanek, P. Koci, M. Marek, and M. Kubicek. Evaluation of local pore sizes and transport properties in porous catalysts. Chem. Eng. Sci., 65(7):2352-2360, 2010. Figure 1
Published: 2021
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50. 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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