Structurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes

Ho-Young Jang, Donggun Eum, Jiung Cho, Jun Lim, Yeji Lee, Jun-Hyuk Song, Hyeokjun Park, Byunghoon Kim, Do-Hoon Kim, Sung-Pyo Cho, Sugeun Jo, Jae Hoon Heo, Sunyoung Lee, Jongwoo Lim and Kisuk Kang ()
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Ho-Young Jang: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Donggun Eum: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Jiung Cho: Seoul Western Center, Korea Basic Science Institute (KBSI)
Jun Lim: Pohang Light Source-II, Pohang University of Science and Technology (POSTECH)
Yeji Lee: Pohang Light Source-II, Pohang University of Science and Technology (POSTECH)
Jun-Hyuk Song: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Hyeokjun Park: Interdisciplinary Materials Measurement Institute, Korea Research Institute of Standards and Science (KRISS)
Byunghoon Kim: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Do-Hoon Kim: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Sung-Pyo Cho: National Center for Inter-University Research Facilities, Seoul National University
Sugeun Jo: College of Science, Seoul National University
Jae Hoon Heo: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Sunyoung Lee: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University
Jongwoo Lim: College of Science, Seoul National University
Kisuk Kang: Institute for Rechargeable Battery Innovations, Research Institute of Advanced Materials, Seoul National University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract O2-type lithium-rich layered oxides, known for mitigating irreversible transition metal migration and voltage decay, provide suitable framework for exploring the inherent properties of oxygen redox. Here, we present a series of O2-type lithium-rich layered oxides exhibiting minimal structural disordering and stable voltage retention even with high anionic redox participation based on the nominal composition. Notably, we observe a distinct asymmetric lattice breathing phenomenon within the layered framework driven by excessive oxygen redox, which includes substantial particle-level mechanical stress and the microcracks formation during cycling. This chemo-mechanical degradation can be effectively mitigated by balancing the anionic and cationic redox capabilities, securing both high discharge voltage (~ 3.43 V vs. Li/Li+) and capacity (~ 200 mAh g−1) over extended cycles. The observed correlation between the oxygen redox capability and the structural evolution of the layered framework suggests the distinct intrinsic capacity fading mechanism that differs from the previously proposed voltage fading mode.

Date: 2024
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DOI: 10.1038/s41467-024-45490-x

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