Jean-Marie Tarascon

Chimie du Solide et Energie

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Gwenaëlle Rousse

Collège de France

Matthieu Saubanère

Université de Montpellier

J. Rodrı́guez-Carvajal

Institut Laue-Langevin

Artem M. Abakumov

Skolkovo Institute of Science and Technology

Michaël Deschamps

Conditions Extrêmes et Matériaux Haute Température et Irradiation

Antonella Iadecola

Réseau sur le Stockage Electrochimique de l'énergie

A. S. Prakash

Central Electrochemical Research Institute

Matthieu Courty

Laboratoire de Réactivité et Chimie des Solides

Sujoy Saha

Institut de Mathématiques de Jussieu-Paris Rive Gauche

Moulay Tahar Sougrati

Réseau sur le Stockage Electrochimique de l'énergie

Cooperative Institutions

Centre National de la Recherche Scientifique

Réseau sur le Stockage Electrochimique de l'énergie

Université de Picardie Jules Verne

Collège de France

Chimie du Solide et Energie

Sorbonne Université

Laboratoire de Réactivité et Chimie des Solides

Energy Storage Systems (United States)

Institut de Chimie

Alistore

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Electrochemical Reactivity of Mg2Sn Phases with Metallic Lithium.

ChemInform (2005)

Dominique Larcher A. S. Prakash Juliette A. Saint Mathieu Morcrette Jean-Marie Tarascon

For Abstract see ChemInform Abstract in Full Text.

Reactivity

Lithium metal

10.1002/chin.200511023

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Citations (0)

Polymorphism in Li₄Zn(PO₄)₂ and Stabilization of its Structural Disorder to Improve Ionic Conductivity

Chemistry of Materials (2018)

Sujoy Saha Gwenaëlle Rousse Ignacio Blazquez Alcover Matthieu Courty Daniel Alves Dalla Corte

Realization of the vulnerability of current rechargeable battery systems drives the research of solid electrolytes. In the search for a new Li ion conductor, we explored the rich crystal chemistry of Li4Zn(PO4)2, which presents a low-temperature monoclinic (α-) and a high-temperature orthorhombic (β-) polymorph. We solved the crystal structure of the β phase and found that it has a disordered Li/Zn-sublattice while showing the largest conductivity; however, it could not be stabilized at room temperature by quenching. We discovered that the partial substitution of Zn2+ with Ga3+ in Li4–xZn1–xGax(PO4)2 first leads to an intermediate β′ phase. Increasing the Ga content to 0.5 mol pfu enables us to stabilize the pure β phase at room temperature, which exhibits a conductivity by several orders of magnitude higher than the pristine sample. The crystal structures of the new β′/β-phases have been solved to elucidate the conduction mechanism, which confirms the high sensitivity of ionic conductivity on disorder.

Orthorhombic crystal system

Monoclinic crystal system

Fast ion conductor

10.1021/acs.chemmater.7b05139

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Citations (16)

Strong Oxygen Participation in the Redox Governing the Structural and Electrochemical Properties of Na-Rich Layered Oxide Na₂IrO₃

Chemistry of Materials (2016)

Arnaud J. Perez Dmitry Batuk Matthieu Saubanère Gwenaëlle Rousse Dominique Foix

The recent revival of the Na-ion battery concept has prompted intense activities in the search for new Na-based layered oxide positive electrodes. The largest capacity to date was obtained for a Na-deficient layered oxide that relies on cationic redox processes only. To go beyond this limit, we decided to chemically manipulate these Na-based layered compounds in a way to trigger the participation of the anionic network. We herein report the electrochemical properties of a Na-rich phase Na2IrO3, which can reversibly cycle 1.5 Na+ per formula unit while not suffering from oxygen release nor cationic migrations. Such large capacities, as deduced by complementary XPS, X-ray/neutron diffraction and transmission electron microscopy measurements, arise from cumulative cationic and anionic redox processes occurring simultaneously at potentials as low as 2.7 V vs Na+/Na. The inability to remove more than 1.5 Na+ is rooted in the formation of an O1-type phase having highly stabilized Na sites as confirmed by DFT calculations, which could rationalize as well the competing metal/oxygen redox processes in Na2IrO3. This work will help to define the most fertile directions in the search for novel high energy Na-rich materials based on more sustainable elements than Ir.

Cationic polymerization

10.1021/acs.chemmater.6b03338

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Citations (154)

Na2-Mn[Fe(CN)6 ] Prussian Blue Analog Cathodes for Na-ion Batteries – from fundamentals to practical demonstration

Energy storage materials (2025)

Zhenying Li Yu Wang François Rabuel Michaël Deschamps Gwenaëlle Rousse

Prussian blue

10.1016/j.ensm.2025.104118

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Unraveling the Structure of Iron(III) Oxalate Tetrahydrate and Its Reversible Li Insertion Capability

Chemistry of Materials (2015)

Hania Ahouari Gwenaëlle Rousse J. Rodrı́guez-Carvajal Moulay Tahar Sougrati Matthieu Saubanère

In the search for better batteries, the quest for new positive electrode materials, which are derived from earth-abundant elements and synthesized through low energy demanding processes, has become an area of interest to the scientific community. Many Li–iron based polyanionic compounds have already been considered for Li ion batteries, but there still remain a large variety of Fe-based polyanionic carboxylate compounds (carbonates, oxalates, malonates, etc.) to be explored, among which Fe2(C2O4)3·nH2O is commercially available, but for which structure and electrochemical reactivity toward Li are lacking. By means of combined X-ray and neutron powder diffraction, we unravel for the first time the structure of Fe2(C2O4)3·4H2O. It adopts a triclinic unit cell with iron atoms being octahedrally coordinated by one water molecule and three oxalate groups, two of them being tetradentate. This arrangement translates into zigzag chains linked one to another through the third oxalate molecule to lead to an opened layered structure into which two additional water molecules are located. Moreover, we demonstrate that it reacts with lithium at an average potential of 3.35 V vs. Li leading to a sustainable capacity of 98 mAh/g. The insertion–extraction of the lithium process follows a biphasic process and involves the Fe3+/Fe2+ redox couple as deduced from in situ X-ray powder diffraction and operando Mössbauer spectroscopy measurements.

Carboxylate

Triclinic crystal system

10.1021/cm5043149

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Citations (36)

Decoupling the effect of vacancies and electropositive cations on the anionic redox processes in Na based P2-type layered oxides

Energy storage materials (2020)

Xue Bai Antonella Iadecola Jean-Marie Tarascon Patrick Rozier

Decoupling (probability)

10.1016/j.ensm.2020.05.032

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Citations (52)

Revealing the Reactivity of the Iridium Trioxide Intermediate for the Oxygen Evolution Reaction in Acidic Media

Chemistry of Materials (2019)

Paul E. Pearce Chunzhen Yang Antonella Iadecola J. Rodrı́guez-Carvajal Gwenaëlle Rousse

The development of efficient water splitting heterogeneous catalysts in acidic media is largely hampered by both the slow kinetics of the oxygen evolution reaction (OER) and the limited stability of the electrocatalyst under these harsh working conditions. At the origin of both the activity and the instability of iridium oxides used as OER catalysts in acid conditions is the formation of high-valence IrOx intermediates such as IrO3. Nevertheless, owing to its reactivity with water, this intermediate was never stabilized, and its electrochemical/chemical behavior was never studied in depth. Here, we report a strategy to stabilize this elusive IrO3 intermediate. Furthermore, we demonstrate that upon reactivity with water, gaseous oxygen is generated, while the intermediate is protonated following the reaction IrO3 + xH2O → H2xIrO3 + x/2O2. The resulting hydrated iridium oxide H2IrO3, which possesses three-dimensional proton intercalation/deintercalation channels, can be considered as an enlightening OER model electrocatalyst in acidic media. Owing to its unique proton insertion ability, we could study a yet ill-described charge compensation mechanism upon OER relying on the bulk reversible exchange of protons, which shows remarkable performances and stability. Indeed, enhanced OER is measured, with a dissolution rate lower than the one measured for the "stellar" IrOx/SrIrO3 catalyst. Such a finding opens the route toward the design of new catalysts enlisting proton insertion that could be competitive for water splitting in acidic media.

Oxygen evolution

Reactivity

Reaction intermediate

Proton Transport

10.1021/acs.chemmater.9b01976

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Citations (79)

Development and implementation of a high temperature electrochemical cell for lithium batteries

Electrochemistry Communications (2006)

David Muñoz‐Rojas Jean‐Bernard Leriche Charles Delacourt Philippe Poizot M. Rosa Palacín

Lithium metal

Atmospheric temperature range