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1. Impact of Surface Chemistry of Silicon Nanoparticles on the Structural and Electrochemical Properties of Si/Ni3.4Sn4 Com-posite Anode for Li-Ion Batteries

Author

Azib, Tahar, Thaury, Claire, Cuevas, Fermin, Leroy, Eric, Jordy, Christian, Marx, Nicolas, and Latroche, Michel

Subjects
Condensed Matter - Materials Science
Abstract

Embedding silicon nanoparticles in an intermetallic matrix is a promising strategy to produce remarkable bulk anode materials for lithium-ion (Li-ion) batteries with low potential, high electrochemical capacity and good cycling stability. These composite materials can be synthetized at a large scale using mechanical milling. However, for Si-Ni3Sn4 composites, milling also induces a chemical reaction between the two components leading to the formation of free Sn and NiSi2, which is detrimental to the performance of the electrode. To prevent this reaction, a modification of the surface chemistry of the silicon has been undertaken. Si nanoparticles coated with a surface layer of either carbon or oxide were used instead of pure silicon. The influence of the coating on the composition, (micro)structure and electrochemical properties of Si-Ni3Sn4 composites is studied and compared with that of pure Si. Si coating strongly reduces the reaction between Si and Ni3Sn4 during milling. Moreover, contrary to pure silicon, Si-coated composites have a plate-like mor-phology in which the surface-modified silicon particles are surrounded by a nanostructured, Ni3Sn4-based matrix leading to smooth potential profiles during electrochemical cycling. The chemical homogeneity of the matrix is more uniform for carbon-coated than for oxygen-coated silicon. As a consequence, different electrochemical behaviors are obtained depending on the surface chemistry, with better lithiation properties for the carbon-covered silicon able to deliver over 500 mAh/g for at least 400 cycles.

Published
2021
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2. Ni-Sn intermetallics as efficient buffering matrix of Si anodes in Li-ion batteries

Author

Azib, Tahar, Bibent, Nicolas, Latroche, Michel, Fischer, Florent, Jumas, Jean-Claude, Olivier-Fourcade, Josette, Jordy, Christian, Lippens, Pierre-Emmanuel, and Cuevas, Fermin

Subjects
Condensed Matter - Materials Science
Abstract

For a successful integration of silicon in high-capacity anodes of Li-ion batteries, its intrinsic capacity decay on cycling due to severe volume swelling should be minimized. In this work, Ni-Sn intermetallics are studied as buffering matrix during reversible lithiation of Si-based anodes. Si/Ni-Sn composites have been synthetized by mechanical milling using C and Al as process control agents. Ni3Sn4, Ni3Sn2 intermetallics and their bi-phasic mixture were used as constituents of the buffering matrix. The structure, composition and morphology of the composites have been analyzed by X-ray diffraction (XRD), 119Sn Transmission M\"ossbauer Spectroscopy (TMS) and scanning electron microscopy (SEM). They consist of ~ 150 nm Si nanoparticles embedded in a multi-phase matrix, the nanostructuration of which improves on increasing the Ni3Sn4 amount. The electrochemical properties of the composites were analyzed by galvanostatic cycling in half-cells. Best results for practical applications are found for the bi-phasic matrix Ni3Sn4-Ni3Sn2 in which Ni3Sn4 is electrochemically active while Ni3Sn2 is inactive. Low capacity loss, 0.04 %/cycle, and high coulombic efficiency, 99.6%, were obtained over 200 cycles while maintaining a high reversible capacity above 500 mAh/g at moderate regime C/5, Comment: 11 pages, 7 figures, 5 tables

Published
2020
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3. Role of silicon and carbon on the structural and electrochemical properties of Si-Ni$_{3.4}$Sn$_4$-Al-C anodes for Li-ion batteries

Author

Azib, Tahar, Thaury, Claire, Fariaut-Georges, Cécile, Hézèque, Thierry, Cuevas, Fermin, Jordy, Christian, and Latroche, Michel

Subjects
Physics - Chemical Physics, Condensed Matter - Materials Science
Abstract

Varying the amounts of silicon and carbon, different composites have been prepared by ball milling of Si, Ni$_{3.4}$Sn$_4$, Al and C. Silicon and carbon contents are varied from 10 to 30 wt.% Si, and 0 to 20 wt.% C. The microstructural and electrochemical properties of the composites have been investigated by X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM) and electrochemical galvanostatic cycling up to 1000 cycles. Impact of silicon and carbon contents on the phase occurrence, electrochemical capacity and cycle-life are compared and discussed. For C-content comprised between 9 and 13 wt.% and Si-content >= 20 wt.%, Si nanoparticles are embedded in a Ni$_{3.4}$Sn$_4$-Al-C matrix which is chemically homogeneous at the micrometric scale. For other carbon contents and low Si-amount (10 wt.%), no homogeneous matrix is formed around Si nanoparticles. When homogenous matrix is formed, both Ni$_3$Sn$_4$ and Si participate to the reversible lithiation mechanism, whereas no reaction between Ni$_3$Sn$_4$ and Li is observed for no homogenous matrix. Moreover, best cycle-life performances are obtained when Si nanoparticles are embedded in a homogenous matrix and Si-content is moderate (<= 20 wt.%). Composites with carbon in the 9-13 wt.% range and 20 wt.% silicon lead to the best balance between capacity and life duration upon cycling. This work experimentally demonstrates that embedding Si in an intermetallic/carbon matrix allows to efficiently accommodate Si volume changes on cycling to ensure long cycle-life.

Published
2020
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4. Incorporation of halogens (Cl, Br, and I) in an Li–P–S–O system for exploring new sulfide solid electrolytes with high conductivity and superior electrochemical performance in solid-state batteries.

Author

Raj, Hari, Neveu, Audric, Jordy, Christian, Pelé, Vincent, and Pralong, Valerie

Abstract

Solid electrolytes (SEs) with high conductivity and better stability against lithium metal are the most important requirements for successful commercialization of solid-state battery (SSB) technology. Therefore, in the search for new SEs with the above-mentioned qualities, halogen elements (Cl, Br, and I) were explored in an Li–P–S–O system to prepare Li10GeP2S12 (LGPS)-structured SEs. Among all the prepared SEs, Li3.3PS3.7O0.3Br0.1 and Li3.3PS3.7O0.3I0.1 compositions showed the highest conductivities of 0.77 mS cm−1 and 0.93 (≈1.0) mS cm−1, respectively, at 25 °C. These compounds also showed superior stability against lithium metal in symmetric and full SSB cells tested with an LiNi0.8Co0.15Al0.05O2 (NCA) cathode and graphite anode. Generally, the instability of sulfide-based SEs in an ambient environment is a major issue, whereas our prepared compounds Li3.3PS3.7O0.3Br0.1 and Li3.3PS3.7O0.3I0.1 showed 5 times higher stability under ambient environment conditions as compared to non-doped Li3.2PS3.7O0.3. In situ EIS study performed on the as-prepared full SSBs and after charge–discharge cycles revealed the contribution of interfacial reactions to impedance. Higher interfacial resistances in the full SSB with the Li-metal anode compared to those with the graphite anode were also revealed. The in situ EIS study confirmed that the Li3.3PS3.7O0.3I0.1 solid electrolyte formed the most stable interface with NCA, graphite and Li metal. Finally, postmortem analysis of the full SSB cell and an SE–Li interfacial study conducted using SEM and elemental mapping revealed morphological changes in the electrodes and electrolytes before and after charge–discharge cycles. In summary, the present work reports new sulfide-based solid electrolytes with high conductivity, better air/moisture stability, and excellent interfacial stability. [ABSTRACT FROM AUTHOR]

Published
2024
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5. Innovative L-band electron paramagnetic resonance investigation of solid-state pouch cell batteries.

Author

Dutoit, Charles-Emmanuel, Soleti, Raffaella, Doux, Jean-Marie, Pelé, Vincent, Boireau, Véronique, Jordy, Christian, Pondaven, Simon, and Vezin, Hervé

Subjects
ELECTRON paramagnetic resonance, MICROWAVE imaging, DENDRITIC crystals, ALUMINUM films, CAVITY resonators
Abstract

Usually, the conventional electron paramagnetic resonance (EPR) spectroscopy and imaging use a microwave cavity operating at X-band, i.e. with an excitation frequency of around 9.6 GHz, and remains the most popular mode in the magnetic characterization of lithium batteries to date. We provide here the first low-frequency EPR investigations for monitoring the metallic lithium structures in the solid-state pouch cell batteries. We show that L band, i.e. a microwave frequency of around 1.01 GHz, is an invaluable method to probe in depth the electrode components through a standard pouch cell using aluminum laminated film for packaging without opening the battery. These results offer a new approach for monitoring the nucleation of micrometric and sub-micrometric lithium particles such as dendritic lithium structures which is an important step in the development of reliable solid-state batteries. [ABSTRACT FROM AUTHOR]

Published
2024
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11. Effect of the boron element in a Li–P–S system.

Author

Neveu, Audric, Raj, Hari, Pelé, Vincent, Jordy, Christian, and Pralong, Valerie

Subjects
SOLID electrolytes, IONIC conductivity, ENERGY storage, CHEMICAL stability, BORON
Abstract

Lithium-ion batteries are nowadays a mature technology for energy storage. However, some safety problems have been identified during their operation in high power applications such as fire incidents in electric vehicles. The most promising solution to improve the safety of lithium-ion batteries is replacing the current organic liquid based electrolytes with solid electrolytes. In this context, new solid electrolytes having chemical and electrochemical stability with high ionic conductivity need to be discovered. Therefore, in the present study, a new LGPS-type structural domain is highlighted for the Li–B–P–S system. Ionic conductivities of up to 10−4 S cm−1 have been achieved for prepared solid electrolytes in the Li–B–P–S system, and higher stability against lithium metal as compared to Li10GeP2S12. These solid electrolytes also show better electrochemical characteristics in all solid-state batteries. [ABSTRACT FROM AUTHOR]

Published
2023
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14. First 18650-format Na-ion cells aging investigation: A degradation mechanism study

Author

European Commission, LabEx STORE-EX, Région Nouvelle-Aquitaine, Agence Nationale de la Recherche (France), Ministerio de Economía y Competitividad (España), Nguyen, Long H. B., Sanz Camacho, Paula, Fondard, Jérémie, Carlier, Dany, Croguennec, Laurence, Palacín, M. Rosa, Ponrouch, Alexandre, Courrèges, Cécile, Dedryvère, Rémi, Trad, Khiem, Jordy, Christian, Genies, Sylvie, Reynier, Yvan, Simonin, Loic, European Commission, LabEx STORE-EX, Région Nouvelle-Aquitaine, Agence Nationale de la Recherche (France), Ministerio de Economía y Competitividad (España), Nguyen, Long H. B., Sanz Camacho, Paula, Fondard, Jérémie, Carlier, Dany, Croguennec, Laurence, Palacín, M. Rosa, Ponrouch, Alexandre, Courrèges, Cécile, Dedryvère, Rémi, Trad, Khiem, Jordy, Christian, Genies, Sylvie, Reynier, Yvan, and Simonin, Loic

Abstract

Several Hard carbon||Na3V2(PO4)2F3 full-cells in 18650-format are assembled to demonstrate the possible use of SIBs in stationary applications. The cell aging process is investigated in two different conditions: (i) continuous cycling at different current rates, and (ii) storage at different states-of-charge at various temperatures. The obtained results reveal that the cell degradation depends strongly on the temperature, current rates applied in cycling conditions, or state-of-charge of the storage test. Under cycling conditions, the continuous sodiation/desodiation may induce significant mechanical deformation, leading to the detachment of active materials from the current collector. Furthermore, the post-mortem analysis shows that reaction rate and aging process are not homogeneous along the electrode roll. The XRD analysis shows that Na3V2(PO4)2F3 structure is robust; nevertheless, the material cannot recover the initial Na+ content as the cycling progresses, which is the main cause for capacity loss in the positive electrode. The solid-electrolyte interphase present on the hard carbon surface was characterised using XPS. The hard carbon electrode cannot be detected during this study, evidencing the formation of a relatively thick (>5 nm) passivating layer composed of carbonate salts and NaF, which are the main products of electrolyte decomposition.

Published
2022

15. First 18650-format Na-ion cells aging investigation: A degradation mechanism study

Author

Nguyen, Long H. B., Sanz Camacho, Paula, Fondard, Jérémie, Carlier, Dany, Croguennec, Laurence, Palacín, Maria Rosa, Ponrouch, Alexandre, Courreges, Cecile, Dedryvère, Rémi, Trad, Khiem, Jordy, Christian, Genies, Sylvie, Reynier, Yvan, Simonin, Loic, European Commission, LabEx STORE-EX, Région Nouvelle-Aquitaine, Agence Nationale de la Recherche (France), Ministerio de Economía y Competitividad (España), Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB), Université de Bordeaux (UB)-Institut Polytechnique de Bordeaux-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire 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), 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), SAFT [Bordeaux], Société des accumulateurs fixes et de traction (SAFT), Advanced Lithium Energy Storage Systems - ALISTORE-ERI (ALISTORE-ERI), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Ciència de Materials de Barcelona (ICMAB), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), VITO/EnergyVille, 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), The RS2E Network for the funding of LHBN's PhD thesis as well as the financial support of Région Nouvelle Aquitaine., MRP and AP acknowledge Ministerio de Economía y Competititivad (Spain) for Severo Ochoa Programme for Centres of Excellence in R&D (SEV-2015-0496)., ANR-10-LABX-0076,STORE-EX,Laboratory of excellency for electrochemical energy storage(2010), and European Project: 646433,H2020,H2020-LCE-2014-3,NAIADES(2015)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Batteries, [CHIM.POLY]Chemical Sciences/Polymers, Renewable Energy, Sustainability and the Environment, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Cycle-life, Cathode materials, Energy Engineering and Power Technology, [CHIM.MATE]Chemical Sciences/Material chemistry, Electrical and Electronic Engineering, Physical and Theoretical Chemistry, Solid-electrolyte interphase
Abstract

Several Hard carbon||Na3V2(PO4)2F3 full-cells in 18650-format are assembled to demonstrate the possible use of SIBs in stationary applications. The cell aging process is investigated in two different conditions: (i) continuous cycling at different current rates, and (ii) storage at different states-of-charge at various temperatures. The obtained results reveal that the cell degradation depends strongly on the temperature, current rates applied in cycling conditions, or state-of-charge of the storage test. Under cycling conditions, the continuous sodiation/desodiation may induce significant mechanical deformation, leading to the detachment of active materials from the current collector. Furthermore, the post-mortem analysis shows that reaction rate and aging process are not homogeneous along the electrode roll. The XRD analysis shows that Na3V2(PO4)2F3 structure is robust; nevertheless, the material cannot recover the initial Na+ content as the cycling progresses, which is the main cause for capacity loss in the positive electrode. The solid-electrolyte interphase present on the hard carbon surface was characterised using XPS. The hard carbon electrode cannot be detected during this study, evidencing the formation of a relatively thick (>5 nm) passivating layer composed of carbonate salts and NaF, which are the main products of electrolyte decomposition., The authors acknowledge the European Commission for funding this work through the H2020 NAIADES project (LCE10-2014, Contract number 646433). LC, DC, PSC and LHBN thank the RS2E Network for the funding of LHBN's PhD thesis as well as the financial support of Région Nouvelle Aquitaine. LC, DC, PSC, LHBN, CC, and RD acknowledge the French National Research Agency (STORE-EX Labex Project ANR-10-LABX-76-01) for financial support. MRP and AP acknowledge Ministerio de Economía y Competititivad (Spain) for Severo Ochoa Programme for Centres of Excellence in R&D (SEV-2015-0496). The authors thank E. Garitte (SAFT, France) for her helps to coordinate this project.

Published
2022
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17. ELECTROLYTES INORGANIQUES MIXTES DE LITHIUM

Author

Pralong, Valérie, Pelé, Vincent, Jordy, Christian, Roumegous, Nadege, Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Normandie Université (NU), and Pralong, Valerie

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry
Published
2021

19. LITHIUM MIXED INORGANIC ELECTROLYTES

Author

Pralong, Valérie, Pelé, Vincent, Jordy, Christian, Rougemous, Nadège, Pralong, Valerie, Normandie Université (NU), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [CHIM.MATE]Chemical Sciences/Material chemistry
Published
2021

25. Study of Graphite Cycling in Sulfide Solid Electrolytes

Author

Höltschi, Laura, primary, Jud, Franziska, additional, Borca, Camelia, additional, Huthwelker, Thomas, additional, Villevieille, Claire, additional, Pelé, Vincent, additional, Jordy, Christian, additional, El Kazzi, Mario, additional, and Novák, Petr, additional

Published
2020
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28. Electrochemical properties of MgH 2 – TiH 2 nanocomposite as active materials for all-solid-state lithium batteries

Author

Dao, Anh Ha, Berti, Nicola, López-Aranguren, Pedro, Zhang, Junxian, Cuevas, Fermin, Jordy, Christian, Latroche, Michel, Latroche, Michel, Institut de Chimie et des Matériaux Paris-Est (ICMPE), Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), SAFT, Direction de la Recherche, Université de Bordeaux (UB), SAFT [Bordeaux], and Société des accumulateurs fixes et de traction (SAFT)

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

29. Sacrificial active material of a positive electrode for a sodium-ion electrochemical element

Author

Pralong, Valérie, Garitte, Emmanuelle, Gillot, S., Jordy, Christian, Adamczyk, Evan, Pralong, Valerie, Institut de Chimie du CNRS (INC), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry
Published
2018

30. Li2O:Li–Mn–O Disordered Rock‐Salt Nanocomposites as Cathode Prelithiation Additives for High‐Energy Density Li‐Ion Batteries.

Author

Diaz‐Lopez, Maria, Chater, Philip A., Bordet, Pierre, Freire, Melanie, Jordy, Christian, Lebedev, Oleg I., and Pralong, Valerie

Subjects
LITHIUM-ion batteries, ADDITIVES, CATHODES, ROCK salt, STORAGE batteries, DENSITY
Abstract

The irreversible loss of lithium from the cathode material during the first cycles of rechargeable Li‐ion batteries notably reduces the overall cell capacity. Here, a new family of sacrificial cathode additives based on Li2O:Li2/3Mn1/3O5/6 composites synthesized by mechanochemical alloying is reported. These nanocomposites display record (but irreversible) capacities within the Li–Mn–O systems studied, of up to 1157 mAh g−1, which represents an increase of over 300% of the originally reported capacity in Li2/3Mn1/3O5/6 disordered rock salts. Such a high irreversible capacity is achieved by the reaction between Li2O and Li2/3Mn1/3O5/6 during the first charge, where electrochemically active Li2O acts as a Li+ donor. A 13% increase of the LiFePO4 and LiCoO2 first charge gravimetric capacities is demonstrated by the addition of only 2 wt% of the nanosized composite in the cathode mixture. This result shows the great potential of these newly discovered sacrificial additives to counteract initial losses of Li+ ions and improve battery performance. [ABSTRACT FROM AUTHOR]

Published
2020
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32. An all-solid-state metal hydride – Sulfur lithium-ion battery

Author

López-Aranguren, Pedro, Berti, Nicola, Dao, Anh Ha, Zhang, Junxian, Cuevas, Fermin, Latroche, Michel, Jordy, Christian, Latroche, Michel, SAFT [Bordeaux], Société des accumulateurs fixes et de traction (SAFT), Institut de Chimie et des Matériaux Paris-Est (ICMPE), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), and Institut de Chimie du CNRS (INC)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

33. Post Mortemand OperandoXPEEM: a Surface-Sensitive Tool for Studying Single Particles in Li-Ion Battery Composite Electrodes

Author

Mirolo, Marta, Leanza, Daniela, Höltschi, Laura, Jordy, Christian, Pelé, Vincent, Novák, Petr, El Kazzi, Mario, and Vaz, Carlos A. F.

Abstract

X-ray photoemission electron microscopy (XPEEM), with its excellent spatial resolution, is a well-suited technique for elucidating the complex electrode–electrolyte interface reactions in Li-ion batteries. It provides element-specific contrast images that allows the study of the surface morphology and the identification of the various components of the composite electrode. It also enables the acquisition of local X-ray absorption spectra (XAS) on single particles of the electrode, such as the C and O K-edges to track the stability of carbonate-based electrolytes, F K-edge to study the electrolyte salt and binder stability, and the transition metal L-edges to gain insights into the oxidation/reduction processes of positive and negative active materials. Here we discuss the optimal measurement conditions for XPEEM studies of Li-ion battery systems, including (i) electrode preparation through mechanical pressing to reduce surface roughness for improved spatial resolution; (ii) corrections of the XAS spectra at the C K-edge to remove the carbon signal contribution originating from the X-ray optics; and (iii) procedures for minimizing the effect of beam damage. Examples from our recent work are provided to demonstrate the strength of XPEEM to solve challenging interface reaction mechanisms via post mortemmeasurements. Finally, we present a first XPEEM cell dedicated to operando/in situexperiments in all-solid-state batteries. Representative measurements were carried out on a graphite electrode cycled with LiI-incorporated sulfide-based electrolyte. This measurement demonstrates the strong competitive reactions between the lithiated graphite surface and the Li2O formation caused by the reaction of the intercalated lithium with the residual oxygen in the vacuum chamber. Moreover, we show the versatility of the operando XPEEM cell to investigate other active materials, for example, Li4Ti5O12.

Published
2020
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39. Spectroscopic Insight into Li-Ion Batteries during Operation: An Alternative Infrared Approach.

Author

Alves Dalla Corte, Daniel, Caillon, Georges, Jordy, Christian, Chazalviel, Jean‐Noël, Rosso, Michel, and Ozanam, François

Subjects
INFRARED spectroscopy, AMORPHOUS silicon, ELECTRODES, LITHIUM-ion batteries, LITHIATION
Abstract

Multiple-internal-reflection infrared spectroscopy allows for the study of thin-film amorphous silicon electrodes in situ and in operando, in conditions typical of those used in Li-ion batteries. It brings an enhanced sensitivity, and the attenuated-total-reflection geometry allows for the extraction of quantitative information. When electrodes are cycled in representative electrolytes, the simultaneously recorded infrared spectra give an insight into the solid/electrolyte interphase (SEI) composition. They also unravel the dynamic behavior of this SEI layer by quantitatively assessing its thickness, which increases during silicon lithiation and partially decreases during delithiation. Li-ion solvation effects in the vicinity of the electrode indicate that lithium incorporation in the solid phase is the rate-determining step of the electrochemical processes during lithiation. The lithiation of the active material also results in the irreversible consumption of a large quantity of hydrogen in the pristine material. Finally, the evolution of the electronic absorption of the electrode material suggests that lithium diffusion is much easier after the first lithiation than in the pristine material. Therefore, in situ Fourier-transform infrared spectroscopy performed in a well-suited configuration efficiently extracts original and quantitative pieces of information on the surface and bulk phenomena affecting Li-ion electrodes during their operation in realistic conditions. [ABSTRACT FROM AUTHOR]

Published
2016
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40. Impact of Surface Chemistry of Silicon Nanoparticles on the Structural and Electrochemical Properties of Si/Ni 3.4 Sn 4 Composite Anode for Li-Ion Batteries.

Author

Azib, Tahar, Thaury, Claire, Cuevas, Fermin, Leroy, Eric, Jordy, Christian, Marx, Nicolas, and Latroche, Michel

Subjects
SURFACE chemistry, SILICON surfaces, NANOSILICON, LITHIUM-ion batteries, ELECTROCHEMICAL electrodes, MECHANICAL alloying, BULK solids
Abstract

Embedding silicon nanoparticles in an intermetallic matrix is a promising strategy to produce remarkable bulk anode materials for lithium-ion (Li-ion) batteries with low potential, high electrochemical capacity and good cycling stability. These composite materials can be synthetized at a large scale using mechanical milling. However, for Si-Ni3Sn4 composites, milling also induces a chemical reaction between the two components leading to the formation of free Sn and NiSi2, which is detrimental to the performance of the electrode. To prevent this reaction, a modification of the surface chemistry of the silicon has been undertaken. Si nanoparticles coated with a surface layer of either carbon or oxide were used instead of pure silicon. The influence of the coating on the composition, (micro)structure and electrochemical properties of Si-Ni3Sn4 composites is studied and compared with that of pure Si. Si coating strongly reduces the reaction between Si and Ni3Sn4 during milling. Moreover, contrary to pure silicon, Si-coated composites have a plate-like morphology in which the surface-modified silicon particles are surrounded by a nanostructured, Ni3Sn4-based matrix leading to smooth potential profiles during electrochemical cycling. The chemical homogeneity of the matrix is more uniform for carbon-coated than for oxygen-coated silicon. As a consequence, different electrochemical behaviors are obtained depending on the surface chemistry, with better lithiation properties for the carbon-covered silicon able to deliver over 500 mAh/g for at least 400 cycles. [ABSTRACT FROM AUTHOR]

Published
2021
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42. Croissance par pulvérisation cathodique d’un nanocomposite LiF-Cu et son application comme positive de batterie au lithium

Author

MUNIER, Antoine, François Weill, Philippe Vinatier, Mario Maglione [Président], Danielle Gonbeau [Rapporteur], Laure Monconduit [Rapporteur], Christian Jordy, Weill, François, Vinatier, Philippe, Jordy, Christian, Maglione, Mario, Gonbeau, Danielle, and Monconduit, Laure

Subjects
Nanocomposite, Électrochimie, Batteries au lithium, Pulvérisation cathodique RF magnétron, Microscopie électronique, Matériaux de conversion, Croissance

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