Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Jin Zhang, Qinchao Wang, Shaofeng Li, Zhisen Jiang, Sha Tan, Xuelong Wang, Kai Zhang, Qingxi Yuan (), Sang-Jun Lee, Charles J. Titus, Kent D. Irwin, Dennis Nordlund, Jun-Sik Lee, Piero Pianetta, Xiqian Yu, Xianghui Xiao, Xiao-Qing Yang, Enyuan Hu () and Yijin Liu ()
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Jin Zhang: Chinese Academy of Science
Qinchao Wang: Brookhaven National Laboratory
Shaofeng Li: SLAC National Accelerator Laboratory
Zhisen Jiang: SLAC National Accelerator Laboratory
Sha Tan: Brookhaven National Laboratory
Xuelong Wang: Brookhaven National Laboratory
Kai Zhang: Chinese Academy of Science
Qingxi Yuan: Chinese Academy of Science
Sang-Jun Lee: SLAC National Accelerator Laboratory
Charles J. Titus: Stanford University
Kent D. Irwin: Stanford University
Dennis Nordlund: SLAC National Accelerator Laboratory
Jun-Sik Lee: SLAC National Accelerator Laboratory
Piero Pianetta: SLAC National Accelerator Laboratory
Xiqian Yu: Chinese Academy of Sciences
Xianghui Xiao: Brookhaven National Laboratory
Xiao-Qing Yang: Brookhaven National Laboratory
Enyuan Hu: Brookhaven National Laboratory
Yijin Liu: SLAC National Accelerator Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li1.2Ni0.13Mn0.54Co0.13O2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles’ core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.

Date: 2020
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DOI: 10.1038/s41467-020-20198-w

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