Understanding voltage decay in lithium-excess layered cathode materials through oxygen-centred structural arrangement

Seungjun Myeong, Woongrae Cho, Wooyoung Jin, Jaeseong Hwang, Moonsu Yoon, Youngshin Yoo, Gyutae Nam, Haeseong Jang, Jung-Gu Han, Nam-Soon Choi, Min Gyu Kim () and Jaephil Cho ()
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Seungjun Myeong: Ulsan National Institute of Science and Technology (UNIST)
Woongrae Cho: Ulsan National Institute of Science and Technology (UNIST)
Wooyoung Jin: Ulsan National Institute of Science and Technology (UNIST)
Jaeseong Hwang: Ulsan National Institute of Science and Technology (UNIST)
Moonsu Yoon: Ulsan National Institute of Science and Technology (UNIST)
Youngshin Yoo: Ulsan National Institute of Science and Technology (UNIST)
Gyutae Nam: Ulsan National Institute of Science and Technology (UNIST)
Haeseong Jang: Ulsan National Institute of Science and Technology (UNIST)
Jung-Gu Han: Ulsan National Institute of Science and Technology (UNIST)
Nam-Soon Choi: Ulsan National Institute of Science and Technology (UNIST)
Min Gyu Kim: Pohang Accelerator Laboratory (PAL)
Jaephil Cho: Ulsan National Institute of Science and Technology (UNIST)

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Lithium-excess 3d-transition-metal layered oxides (Li1+xNiyCozMn1−x−y−zO2, >250 mAh g−1) suffer from severe voltage decay upon cycling, which decreases energy density and hinders further research and development. Nevertheless, the lack of understanding on chemical and structural uniqueness of the material prevents the interpretation of internal degradation chemistry. Here, we discover a fundamental reason of the voltage decay phenomenon by comparing ordered and cation-disordered materials with a combination of X-ray absorption spectroscopy and transmission electron microscopy studies. The cation arrangement determines the transition metal-oxygen covalency and structural reversibility related to voltage decay. The identification of structural arrangement with de-lithiated oxygen-centred octahedron and interactions between octahedrons affecting the oxygen stability and transition metal mobility of layered oxide provides the insight into the degradation chemistry of cathode materials and a way to develop high-energy density electrodes.

Date: 2018
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DOI: 10.1038/s41467-018-05802-4

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