Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries

Shuaifeng Lou, Qianwen Liu, Fang Zhang, Qingsong Liu, Zhenjiang Yu, Tiansheng Mu, Yang Zhao, James Borovilas, Yijun Chen, Mingyuan Ge, Xianghui Xiao, Wah-Keat Lee, Geping Yin, Yuan Yang, Xueliang Sun and Jiajun Wang ()
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Shuaifeng Lou: Harbin Institute of Technology
Qianwen Liu: Harbin Institute of Technology
Fang Zhang: Harbin Institute of Technology
Qingsong Liu: Harbin Institute of Technology
Zhenjiang Yu: Harbin Institute of Technology
Tiansheng Mu: Harbin Institute of Technology
Yang Zhao: University of Western Ontario
James Borovilas: Columbia University
Yijun Chen: Columbia University
Mingyuan Ge: National Synchrotron Light Source II, Brookhaven National Laboratory
Xianghui Xiao: National Synchrotron Light Source II, Brookhaven National Laboratory
Wah-Keat Lee: National Synchrotron Light Source II, Brookhaven National Laboratory
Geping Yin: Harbin Institute of Technology
Yuan Yang: Columbia University
Xueliang Sun: University of Western Ontario
Jiajun Wang: Harbin Institute of Technology

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Interfacial issues commonly exist in solid-state batteries, and the microstructural complexity combines with the chemical heterogeneity to govern the local interfacial chemistry. The conventional wisdom suggests that “point-to-point” ion diffusion at the interface determines the ion transport kinetics. Here, we show that solid-solid ion transport kinetics are not only impacted by the physical interfacial contact but are also closely associated with the interior local environments within polycrystalline particles. In spite of the initial discrete interfacial contact, solid-state batteries may still display homogeneous lithium-ion transportation owing to the chemical potential force to achieve an ionic-electronic equilibrium. Nevertheless, once the interior local environment within secondary particle is disrupted upon cycling, it triggers charge distribution from homogeneity to heterogeneity and leads to fast capacity fading. Our work highlights the importance of interior local environment within polycrystalline particles for electrochemical reactions in solid-state batteries and provides crucial insights into underlying mechanism in interfacial transport.

Date: 2020
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DOI: 10.1038/s41467-020-19528-9

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