Unlocking the passivation nature of the cathode–air interfacial reactions in lithium ion batteries

Lianfeng Zou, Yang He, Zhenyu Liu, Haiping Jia, Jian Zhu, Jianming Zheng, Guofeng Wang, Xiaolin Li, Jie Xiao, Jun Liu, Ji-Guang Zhang, Guoying Chen and Chongmin Wang ()
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Lianfeng Zou: Pacific Northwest National Laboratory
Yang He: Pacific Northwest National Laboratory
Zhenyu Liu: University of Pittsburgh
Haiping Jia: Pacific Northwest National Laboratory
Jian Zhu: Lawrence Berkeley National Laboratory
Jianming Zheng: Pacific Northwest National Laboratory
Guofeng Wang: University of Pittsburgh
Xiaolin Li: Pacific Northwest National Laboratory
Jie Xiao: Pacific Northwest National Laboratory
Jun Liu: Pacific Northwest National Laboratory
Ji-Guang Zhang: Pacific Northwest National Laboratory
Guoying Chen: Lawrence Berkeley National Laboratory
Chongmin Wang: Pacific Northwest National Laboratory

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

Abstract: Abstract It is classically well perceived that cathode–air interfacial reactions, often instantaneous and thermodynamic non-equilibrium, will lead to the formation of interfacial layers, which subsequently, often vitally, control the behaviour and performance of batteries. However, understanding of the nature of cathode–air interfacial reactions remain elusive. Here, using atomic-resolution, time-resolved in-situ environmental transmission electron microscopy and atomistic simulation, we reveal that the cathode–water interfacial reactions can lead to the surface passivation, where the resultant conformal LiOH layers present a critical thickness beyond which the otherwise sustained interfacial reactions are arrested. We rationalize that the passivation behavior is dictated by the Li+-water interaction driven Li-ion de-intercalation, rather than a direct cathode–gas chemical reaction. Further, we show that a thin disordered rocksalt layer formed on the cathode surface can effectively mitigate the surface degradation by suppressing chemical delithiation. The established passivation paradigm opens new venues for the development of novel high-energy and high-stability cathodes.

Date: 2020
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DOI: 10.1038/s41467-020-17050-6

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