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

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

doi:10.1038/s41467-020-14927-4

Title: Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li_1.2Ni_0.13Mn_0.54Co_0.13O₂

Journal Article · Fri Mar 06 00:00:00 EST 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-14927-4· OSTI ID:1631047

^[1];

^[1]; Rousse, Gwenaelle ^[1]; Abakumov, Artem M. ^[2]; Senyshyn, Anatoliy ^[3]; Zhang, Leiting ^[4];

^[4]; Iadecola, Antonella ^[5]; Foix, Dominique ^[6]; Giaume, Domitille ^[7];

^[1]

Collège de France (France); Sorbonne Université, 4 Place Jussieu, 75005, Paris, France; Sorbonne Univ., Paris (France); National Centre for Scientific Research-Mixed Organizations (CNRS-UMR), Paris (France)
Skolkovo Inst. of Science and Technology, Moscow (Russia)
Technische Univ. Munchen, Garching (Germany)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Sorbonne Univ., Paris (France); National Centre for Scientific Research-Mixed Organizations (CNRS-UMR), Paris (France)
National Centre for Scientific Research-Mixed Organizations (CNRS-UMR), Paris (France)
National Centre for Scientific Research (CNRS), Paris (France)

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 Li_1.2Ni_0.13Mn_0.54Co_0.13O₂ 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 Li_1.2Ni_0.13Mn_0.54Co_0.13O₂ and will help to find measures to cure voltage fade and improve energy efficiency in this class of material.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1631047

Journal Information:: Nature Communications, Vol. 11, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 74 works

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

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Title: Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li_1.2Ni_0.13Mn_0.54Co_0.13O₂