Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2

Wei Yin; Alexis Grimaud; Gwenaëlle Rousse; Artem Abakumov; Anatoliy Senyshyn; Leiting Zhang; Sigita Trabesinger; Antonella Iadecola; Dominique Foix; Domitille Giaume; Jean-Marie Tarascon

doi:10.1038/s41467-020-14927-4

Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2

Wei Yin ¹ Alexis Grimaud ² Gwenaëlle Rousse ³ Artem Abakumov ⁴ Anatoliy Senyshyn ⁵ Leiting Zhang ⁶ Sigita Trabesinger Antonella Iadecola ⁷ Dominique Foix ^{8, 9} Domitille Giaume ¹⁰ Jean-Marie Tarascon ^{3, 1, *}

* Corresponding author

1 Chimie du solide et de l'énergie

2 RS2E - Réseau sur le stockage électrochimique de l'énergie

3 Sorbonne Universités

4 Skoltech - Skolkovo Institute of Science and Technology [Moscow]

5 TUM - Technical University of Munich

6 PSI - Paul Scherrer Institute

7 SSOLEIL - Synchrotron SOLEIL

8 Advanced Lithium Energy Storage Systems - ALISTORE (FRANCE)

9 IPREM - Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux

10 LPMC - Laboratoire de physique de la matière condensée

Abstract : High-energy-density lithium-rich materials are of significant interest for advanced lithium-ion batteries, provided that several roadblocks, such as voltage fade and poor energy efficiency are removed. However, this remains challenging as their functioning mechanisms during first cycle are not fully understood. Here we enlarge the cycling potential window for Li1.2Ni0.13Mn0.54Co0.13O2 electrode, identifying novel structural evolution mechanism involving a structurally-densified single-phase A’ formed under harsh oxidizing conditions throughout the crystallites and not only at the surface, in contrast to previous beliefs. We also recover a majority of first-cycle capacity loss by applying a constant-voltage step on discharge. Using highly reducing conditions we obtain additional capacity via a new low-potential P” phase, which is involved into triggering oxygen redox on charge. Altogether, these results provide deeper insights into the structural-composition evolution of Li1.2Ni0.13Mn0.54Co0.13O2 and will help to find measures to cure voltage fade and improve energy efficiency in this class of material.

Keywords : battery

Document type :

Journal articles

Domain :

Chemical Sciences / Polymers

Chemical Sciences / Material chemistry

Chemical Sciences / Theoretical and/or physical chemistry

Chemical Sciences / Analytical chemistry

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Submitted on : Monday, March 23, 2020 - 12:39:54 PM
Last modification on : Wednesday, March 25, 2020 - 1:14:48 AM

Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2

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Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2

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