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1. Understanding Battery Interfaces by Combined Characterization and Simulation Approaches : Challenges and Perspectives

Author

Duncan Atkins, Elixabete Ayerbe, Anass Benayad, Federico G. Capone, Ennio Capria, Ivano E. Castelli, Isidora Cekic‐Laskovic, Raul Ciria, Lenart Dudy, Kristina Edström, Mark R. Johnson, Hongjiao Li, Juan Maria Garcia Lastra, Matheus Leal De Souza, Valentin Meunier, Mathieu Morcrette, Harald Reichert, Patrice Simon, Jean‐Pascal Rueff, Jonas Sottmann, Wolfgang Wenzel, Alexis Grimaud, Institut Laue-Langevin (ILL), CIDETEC, Département des Technologies des NanoMatériaux (DTNM), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), European Synchroton Radiation Facility [Grenoble] (ESRF), Danmarks Tekniske Universitet = Technical University of Denmark (DTU), Forschungszentrum Jülich GmbH, Department of Materials Chemistry - The Angstrom Laboratory, Uppsala University, Max Planck Institute for Meteorology (MPI-M), Max-Planck-Gesellschaft, Réseau sur le stockage électrochimique de l'énergie (RS2E), Aix Marseille Université (AMU)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Nantes Université (Nantes Univ)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Laboratoire réactivité et chimie des solides - UMR CNRS 7314 (LRCS), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Universität für Bodenkultur Wien = University of Natural Resources and Life [Vienne, Autriche] (BOKU), Collège de France - Chaire Chimie du solide et énergie, Chimie du solide et de l'énergie (CSE), and Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Technology, battery interfaces, solid interphases formation, Renewable Energy, Sustainability and the Environment, 020209 energy, Materialkemi, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, 021001 nanoscience & nanotechnology, 7. Clean energy, multiscale modeling, electrochemical analysis, 0202 electrical engineering, electronic engineering, information engineering, Materials Chemistry, General Materials Science, 0210 nano-technology, ddc:600, operando characterization
Abstract

International audience; Driven by the continuous search for improving performances, understanding the phenomena at the electrode/electrolyte interfaces has become an overriding factor for the success of sustainable and efficient battery technologies for mobile and stationary applications. Toward this goal, rapid advances have been made regarding simulations/modeling techniques and characterization approaches, including high-throughput electrochemical measurements coupled with spectroscopies. Focusing on Li-ion batteries, current developments are analyzed in the field as well as future challenges in order to gain a full description of interfacial processes across multiple length/timescales; from charge transfer to migration/diffusion properties and interphases formation, up to and including their stability over the entire battery lifetime. For such complex and interrelated phenomena, developing a unified workflow intimately combining the ensemble of these techniques will be critical to unlocking their full investigative potential. For this paradigm shift in battery design to become reality, it necessitates the implementation of research standards and protocols, underlining the importance of a concerted approach across the community. With this in mind, major collaborative initiatives gathering complementary strengths and skills will be fundamental if societal and environmental imperatives in this domain are to be met. \textcopyright 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH

Published
2022
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2. Combined Operando High Resolution SANS and Neutron Imaging Reveals in-Situ Local Water Distribution in an Operating Fuel Cell

Author

Sylvie Escribano, Nicolas Martinez, Gérard Gebel, Arnaud Morin, Lionel Porcar, Sébastien Rosini, Sandrine Lyonnard, Duncan Atkins, Alessandro Tengattini, Fabrice Micoud, Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Institut Laue-Langevin (ILL), Département de l'Electricité et de l'Hydrogène pour les Transports (DEHS), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), 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), Université Grenoble Alpes (UGA), Département des Technologies des NanoMatériaux (DTNM), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), ILL, Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de L'Energie Solaire (INES), and Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)

Subjects
In situ, Materials science, Hydrogen, Neutron imaging, Energy Engineering and Power Technology, High resolution, Proton exchange membrane fuel cell, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, 0104 chemical sciences, Chemical engineering, chemistry, Yield (chemistry), [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Materials Chemistry, Electrochemistry, Chemical Engineering (miscellaneous), Fuel cells, Electrical and Electronic Engineering, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

By producing electricity and heat from hydrogen with high yield and with only water as a byproduct, the proton exchange membrane fuel cell (PEMFC) is one of the most promising carbon-free alternati...

Published
2019
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3. Neutron imaging of operando proton exchange membrane fuel cell with novel membrane

Author

Alessandro Tengattini, Cristina Iojoiu, Huu-Dat Nguyen, Duncan Atkins, Sébastien Rosini, Fabrice Micoud, Arnaud Morin, Sandrine Lyonnard, Sylvie Escribano, Gérard Gebel, Jongmin Lee, Commissariat à l'énergie atomique et aux énergies alternatives (CEA), 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), Institut Laue-Langevin (ILL), ILL, Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)

Subjects
Materials science, Energy Engineering and Power Technology, Proton exchange membrane fuel cell, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, law.invention, chemistry.chemical_compound, law, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, Ionomer, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, Renewable Energy, Sustainability and the Environment, Neutron imaging, Polymer, 021001 nanoscience & nanotechnology, Cathode, 0104 chemical sciences, Anode, Membrane, [CHIM.POLY]Chemical Sciences/Polymers, chemistry, Chemical engineering, 0210 nano-technology, Current density
Abstract

The performance of an alternative membrane based on aromatic multiblock copolymer was compared to that of the conventional perfluorosulfonic acid (PFSA) polymer membrane during fuel cell operation. The fuel cell with the alternative membrane exhibited more severe voltage loss than the conventional at current densities above 0.6 A/cm2 with fully saturated reactants. To rationalize this difference, operando high-resolution neutron imaging was used to investigate water distribution in the fuel cells, in parallel with impedance measurements. The type of membrane strongly affected water distribution, not only from anode to cathode, but also in-plane between ribs and channels. Specifically, in the alternative membrane, ionomer in cathode catalyst layer was less hydrated and dried as current density increased. The voltage loss with the alternative membrane was ascribed to ionomer drying rather than to the accumulation of liquid water, in accordance with the evolution of ohmic resistance. Furthermore, the alternative membrane experienced swell/shrinkage resulting in material shifts during the operation. These results pinpoint that developing new ionomers for fuel cells require not only to quantify the bulk transport properties of alternative membranes compared to PFSA, but also to evaluate their interfacial properties and the impact of ionomer on water management.

Published
2021
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4. PSI ‘Neutron Microscope’ at ILL-D50 Beamline - First Results

Author

Eberhard Lehmann, Michael Meyer, Markus Strobl, Tengattini Alessandro, Duncan Atkins, Timon Wehmann, and Pavel Trtik

Subjects
Optics, Materials science, Beamline, business.industry, business, Neutron microscope
Abstract

A high-resolution neutron imaging system referred to as ‘Neutron Microscope’ (NM) has been recently established as a piece of instrumental equipment at the Paul Scherrer Institut (PSI), Switzerland. It is providing the wide user community of the Neutron Imaging and Applied Materials Group (NIAG) with the capability of spatial image resolution below 5 µm at effective pixel sizes of 1.3 m. The NM has been designed as a portable, self-contained system that can be moved between beamlines at PSI with only moderate effort. In this contribution, we report on the first results and experience with the Neutron Microscope externally, at a beamline of another neutron source outside the Swiss Spallation Neutron Source (SINQ). In June 2018, NM has been transported to the Institute Laue-Langevin (ILL) and was successfully installed at the D50 beamline for four days. A gadolinium based Siemens star produced at PSI has been used for the assessment of the spatial resolution. The spatial resolution achieved using the Neutron Microscope at ILL-D50 equalled 4.5 µm. Above that, several high-resolution tomographies of various samples were acquired, of which an illustrative example is presented.

Published
2020
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6. Liquid water uptake in unconfined Callovo Oxfordian clay-rock studied with neutron and x-ray imaging

Author

Duncan Atkins, Frédéric Dufour, Eleni Stavropoulou, Alessandro Tengattini, Gilles Armand, Matthieu Briffaut, Edward Andò, Laboratoire sols, solides, structures - risques [Grenoble] (3SR ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Risques, Vulnérabilité des structures et comportement mécanique des matériaux (RV ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), GéoMécanique, Institut Laue-Langevin (ILL), ILL, and Agence Nationale pour la Gestion des Déchets Radioactifs (ANDRA)

Subjects
Materials science, Suction, Capillary action, Neutron imaging, Effective stress, 010102 general mathematics, 0211 other engineering and technologies, Mineralogy, Fracture mechanics, 02 engineering and technology, Geotechnical Engineering and Engineering Geology, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, [PHYS.MECA.MEMA]Physics [physics]/Mechanics [physics]/Mechanics of materials [physics.class-ph], Cracking, [PHYS.MECA.SOLID]Physics [physics]/Mechanics [physics]/Solid mechanics [physics.class-ph], Earth and Planetary Sciences (miscellaneous), [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Neutron, Tomography, 0101 mathematics, [PHYS.COND.CM-SM]Physics [physics]/Condensed Matter [cond-mat]/Statistical Mechanics [cond-mat.stat-mech], 021101 geological & geomatics engineering
Abstract

International audience; The Callovo Oxfordian clay-rock (COx) is studied in France for the disposal of radioactive waste, because of its extremely low permeability. This host rock is governed by a hydromechanical coupling of high complexity.This paper presents an experimental study into the mechanisms of water uptake in small, unconfined, prismatic specimens of COx, motivated by the comprehension of cracking observed during concrete/COx interface sample preparation. Water uptake is monitored using both x-ray tomography and neutron radiography, the combination of these imaging techniques allowing material deformation and water arrival to be quantified respectively.Given the speed of water entry and crack propagation, relatively fast imaging is required: 5 minute x-ray tomographies and ten-second neutron radiographies are used. In this study, pairs of similar COx samples from the same core are tested separately with each imaging technique. Two different orientations with respect to the core are also investigated. Analysis of the resulting images yields with micro-and macro-scale insights into hydro-mechanical mechanisms to be obtained. This allows the cracking to be interpreted as a rapid breakdown in capillary suction (supposed large both to drying and rebound from in-situ stress state) due to water arrival, which in turn causes a loss of effective stress, allowing cracks to propagate with ease, which in turn deliver water further into the material.

Published
2018
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