Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2.
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Yin W
Chimie du Solide et de l'Energie, UMR 8260, Collège de France, 75231, Paris Cedex 05, France.
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Grimaud A
Chimie du Solide et de l'Energie, UMR 8260, Collège de France, 75231, Paris Cedex 05, France.
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Rousse G
Chimie du Solide et de l'Energie, UMR 8260, Collège de France, 75231, Paris Cedex 05, France.
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Abakumov AM
Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, 3 Nobel Street, Moscow, 143026, Russia.
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Senyshyn A
Forschungsneutronenquelle Heinz Maier-Leibnitz (FRM II), Technische Universität München, Lichtenbergstrasse 1, 85748, Garching, Germany.
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Zhang L
Electrochemistry Laboratory, Paul Scherrer Institute, Forschungsstrasse 111, 5232, Villigen PSI, Switzerland.
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Trabesinger S
Electrochemistry Laboratory, Paul Scherrer Institute, Forschungsstrasse 111, 5232, Villigen PSI, Switzerland.
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Iadecola A
Réseau sur le Stockage Electrochimique de l'Energie (RS2E), CNRS FR 3459, 33 Rue Saint Leu, 80039, Amiens, France.
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Foix D
IPREM - UMR 5254 CNRS, Université de Pau et des Pays de l'Adour, Hélioparc, Avenue Pierre Angot, 64053, Pau Cedex 9, France.
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Giaume D
Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie Paris, 75005, Paris, France.
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Tarascon JM
Chimie du Solide et de l'Energie, UMR 8260, Collège de France, 75231, Paris Cedex 05, France. jean-marie.tarascon@college-de-france.fr.
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Published in:
- Nature communications. - 2020
English
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.
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Language
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Open access status
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gold
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Persistent URL
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https://folia.unifr.ch/global/documents/77416
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