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

1. 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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2. 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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3. 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

4. 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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5. 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

6. 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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7. 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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8. 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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9. 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

10. 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

11. 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

12. 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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13. 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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14. 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

15. 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

16. 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

17. 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

18. 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
Full Text
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19. 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

20. 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
Full Text
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21. 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

22. 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

23. 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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24. 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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25. 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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26. 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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27. A chemical-mechanical ex-situ aging of perfluorosulfonic-acid membranes for fuel cells: Impact on the structure and the functional properties

Author

Mylène Robert, Assma El Kaddouri, Marie Crouillere, Jean-Christophe Perrin, Laetitia Dubau, Florence Dubelley, Kévin Mozet, Meriem Daoudi, Jérôme Dillet, Jean-Yves Morel, Sébastien Leclerc, 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), and Electrochimie Interfaciale et Procédés (EIP)

Subjects
Mechanical fatigue, Renewable Energy, Sustainability and the Environment, [SPI.FLUID]Engineering Sciences [physics]/Reactive fluid environment, Water mobility, 05 social sciences, Energy Engineering and Power Technology, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, 021001 nanoscience & nanotechnology, Chemical degradation, Durability, [CHIM.POLY]Chemical Sciences/Polymers, [CHIM.GENI]Chemical Sciences/Chemical engineering, Water sorption, 0502 economics and business, [SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, Nafion ™ membrane, 050207 economics, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, [CHIM.OTHE]Chemical Sciences/Other, 0210 nano-technology
Abstract

International audience; Perfluorosulfonic acid (PFSA) membranes are key components for the operation of Polymer Electrolyte Membrane Fuel Cells (PEMFC). They undergo harsh conditions in terms of chemical environment and mechanical fatigue leading to irreversible degradations, up to their failure and to the Fuel Cell (FC) shutdown in worst cases. Through an ex-situ approach, this study aims to provide new insights about the impact of conjoint mechanical and chemical stresses on the structure and the functional properties of PFSA membranes. In this regard, various aging tests have been carried out using a custom-made device able to combine the application of a mechanical stress (sinusoidal profile) and the exposure to an environment containing free radicals (i.e. Fenton's reagents). After about twenty hours of accelerated aging test the analysis of the aged membranes permitted to demonstrate that the exposure to the combined stress significantly altered the morphology of Nafion ™ XL membrane, with the appearance of bubbles close to the membrane surface and even delamination at the PFSA/reinforcement interface. On the other hand, and rather paradoxically, the water sorption and self-diffusion properties of the aged membranes as well as their cell performances remained satisfactory.

Published
2022
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