In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

Longlong Wang, Ruicong Xie, Bingbing Chen, Xinrun Yu, Jun Ma (), Chao Li (), Zhiwei Hu, Xingwei Sun, Chengjun Xu, Shanmu Dong, Ting-Shan Chan, Jun Luo (), Guanglei Cui () and Liquan Chen
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Longlong Wang: Chinese Academy of Sciences
Ruicong Xie: Tianjin University of Technology
Bingbing Chen: Nanjing Tech University
Xinrun Yu: Chinese Academy of Sciences
Jun Ma: Chinese Academy of Sciences
Chao Li: Tianjin University of Technology
Zhiwei Hu: Max Plank Institute for Chemical Physics of Solids
Xingwei Sun: Chinese Academy of Sciences
Chengjun Xu: Nanjing Tech University
Shanmu Dong: Chinese Academy of Sciences
Ting-Shan Chan: National Synchrotron Radiation Research Center
Jun Luo: Tianjin University of Technology
Guanglei Cui: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract The space charge layer (SCL) is generally considered one of the origins of the sluggish interfacial lithium-ion transport in all-solid-state lithium-ion batteries (ASSLIBs). However, in-situ visualization of the SCL effect on the interfacial lithium-ion transport in sulfide-based ASSLIBs is still a great challenge. Here, we directly observe the electrode/electrolyte interface lithium-ion accumulation resulting from the SCL by investigating the net-charge-density distribution across the high-voltage LiCoO2/argyrodite Li6PS5Cl interface using the in-situ differential phase contrast scanning transmission electron microscopy (DPC-STEM) technique. Moreover, we further demonstrate a built-in electric field and chemical potential coupling strategy to reduce the SCL formation and boost lithium-ion transport across the electrode/electrolyte interface by the in-situ DPC-STEM technique and finite element method simulations. Our findings will strikingly advance the fundamental scientific understanding of the SCL mechanism in ASSLIBs and shed light on rational electrode/electrolyte interface design for high-rate performance ASSLIBs.

Date: 2020
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DOI: 10.1038/s41467-020-19726-5

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