Reaction inhomogeneity coupling with metal rearrangement triggers electrochemical degradation in lithium-rich layered cathode

Liguang Wang, Tongchao Liu, Alvin Dai, Vincent Andrade, Yang Ren, Wenqian Xu, Sungsik Lee, Qinghua Zhang, Lin Gu, Shun Wang, Tianpin Wu (), Huile Jin () and Jun Lu ()
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Liguang Wang: Wenzhou University
Tongchao Liu: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Vincent Andrade: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Wenqian Xu: Argonne National Laboratory
Sungsik Lee: Argonne National Laboratory
Qinghua Zhang: Chinese Academy of Science
Lin Gu: Chinese Academy of Science
Shun Wang: Wenzhou University
Tianpin Wu: Argonne National Laboratory
Huile Jin: Wenzhou University
Jun Lu: Argonne National Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract High-energy density lithium-rich layered oxides are among the most promising candidates for next-generation energy storage. Unfortunately, these materials suffer from severe electrochemical degradation that includes capacity loss and voltage decay during long-term cycling. Present research efforts are primarily focused on understanding voltage decay phenomena while origins for capacity degradation have been largely ignored. Here, we thoroughly investigate causes for electrochemical performance decline with an emphasis on capacity loss in the lithium-rich layered oxides, as well as reaction pathways and kinetics. Advanced synchrotron-based X-ray two-dimensional and three-dimensional imaging techniques are combined with spectroscopic and scattering techniques to spatially visualize the reactivity at multiple length-scales on lithium- and manganese-rich layered oxides. These methods provide direct evidence for inhomogeneous manganese reactivity and ionic nickel rearrangement. Coupling deactivated manganese with nickel migration provides sluggish reaction kinetics and induces serious structural instability in the material. Our findings provide new insights and further understanding of electrochemical degradation, which serve to facilitate cathode material design improvements.

Date: 2021
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DOI: 10.1038/s41467-021-25686-1

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