Origin of structural degradation in Li-rich layered oxide cathode

Tongchao Liu, Jiajie Liu, Luxi Li, Lei Yu, Jiecheng Diao, Tao Zhou, Shunning Li, Alvin Dai, Wenguang Zhao, Shenyang Xu, Yang Ren, Liguang Wang, Tianpin Wu, Rui Qi, Yinguo Xiao, Jiaxin Zheng, Wonsuk Cha, Ross Harder, Ian Robinson, Jianguo Wen, Jun Lu (), Feng Pan () and Khalil Amine ()
Additional contact information
Tongchao Liu: Argonne National Laboratory
Jiajie Liu: Peking University, Shenzhen Graduate School
Luxi Li: Argonne National Laboratory
Lei Yu: Argonne National Laboratory
Jiecheng Diao: University College London
Tao Zhou: Argonne National Laboratory
Shunning Li: Peking University, Shenzhen Graduate School
Alvin Dai: Argonne National Laboratory
Wenguang Zhao: Peking University, Shenzhen Graduate School
Shenyang Xu: Peking University, Shenzhen Graduate School
Yang Ren: Argonne National Laboratory
Liguang Wang: Argonne National Laboratory
Tianpin Wu: Argonne National Laboratory
Rui Qi: Peking University, Shenzhen Graduate School
Yinguo Xiao: Peking University, Shenzhen Graduate School
Jiaxin Zheng: Peking University, Shenzhen Graduate School
Wonsuk Cha: Argonne National Laboratory
Ross Harder: Argonne National Laboratory
Ian Robinson: University College London
Jianguo Wen: Argonne National Laboratory
Jun Lu: Argonne National Laboratory
Feng Pan: Peking University, Shenzhen Graduate School
Khalil Amine: Argonne National Laboratory

Nature, 2022, vol. 606, issue 7913, 305-312

Abstract: Abstract Li- and Mn-rich (LMR) cathode materials that utilize both cation and anion redox can yield substantial increases in battery energy density1–3. However, although voltage decay issues cause continuous energy loss and impede commercialization, the prerequisite driving force for this phenomenon remains a mystery3–6 Here, with in situ nanoscale sensitive coherent X-ray diffraction imaging techniques, we reveal that nanostrain and lattice displacement accumulate continuously during operation of the cell. Evidence shows that this effect is the driving force for both structure degradation and oxygen loss, which trigger the well-known rapid voltage decay in LMR cathodes. By carrying out micro- to macro-length characterizations that span atomic structure, the primary particle, multiparticle and electrode levels, we demonstrate that the heterogeneous nature of LMR cathodes inevitably causes pernicious phase displacement/strain, which cannot be eliminated by conventional doping or coating methods. We therefore propose mesostructural design as a strategy to mitigate lattice displacement and inhomogeneous electrochemical/structural evolutions, thereby achieving stable voltage and capacity profiles. These findings highlight the significance of lattice strain/displacement in causing voltage decay and will inspire a wave of efforts to unlock the potential of the broad-scale commercialization of LMR cathode materials.

Date: 2022
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DOI: 10.1038/s41586-022-04689-y

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