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

Wei Yin, Alexis Grimaud, Gwenaelle Rousse, Artem M. Abakumov, Anatoliy Senyshyn, Leiting Zhang, Sigita Trabesinger, Antonella Iadecola, Dominique Foix, Domitille Giaume and Jean-Marie Tarascon ()
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Wei Yin: Collège de France
Alexis Grimaud: Collège de France
Gwenaelle Rousse: Collège de France
Artem M. Abakumov: Skolkovo Institute of Science and Technology
Anatoliy Senyshyn: Technische Universität München
Leiting Zhang: Paul Scherrer Institute
Sigita Trabesinger: Paul Scherrer Institute
Antonella Iadecola: CNRS FR 3459
Dominique Foix: Université de Pau et des Pays de l’Adour
Domitille Giaume: Institut de Recherche de Chimie Paris
Jean-Marie Tarascon: Collège de France

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-14927-4

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