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, Liquan Chen

Research output: Contribution to journalArticlepeer-review

210 Scopus citations

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.

Original languageEnglish
Article number5889
JournalNature Communications
Volume11
Issue number1
DOIs
StatePublished - 18 Nov 2020
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2020, The Author(s).

Funding

This work was supported by the National Key R&D Program of China (2018YFB0104300), the National Natural Science Foundation of China (21975274, U1706229, 11604241, 51971157, 21603161, 61705115, 11902144, 51971157, and 51761165012), the Young Elite Scientists Sponsorship Program by Tianjin, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA22010600), the National Natural Science Foundation for Distinguished Young Scholars of China (51625204), the Youth Innovation Promotion Association of CAS (2016193), the Key Research and Development Plan of Shandong Province, China (2018GGX104016), the Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), the Tianjin Municipal Science and Technology Commission (19JCQNJC15100), the National Program for Thousand Young Talents of China, DICP & QIBEBT Fund (Grant No. DICP and QIBEBT UN201707) and QIBEBT (ZZBS201808). The authors gratefully acknowledge Prof. Shuping Pang (Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China), Prof. Lin Gu and Dr. Qinghua Zhang (Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China) for the valuable discussions and kind help in revising the manuscript.

FundersFunder number
National Key R&D Program of China2018YFB0104300
Key Technology Research and Development Program of Shandong2018GGX104016
Natural Science Foundation for Distinguished Young Scholars of Anhui Province51625204
National Natural Science Foundation of ChinaU1706229, 21975274, 11604241, 21603161, 51761165012, 61705115, 11902144, 51971157
Chinese Academy of SciencesXDA22010600
Dalian Institute of Chemical PhysicsQIBEBT UN201707, ZZBS201808
Tianjin Science and Technology Committee19JCQNJC15100
Youth Innovation Promotion Association2016193
National Science Fund for Distinguished Young Scholars19JCJQJC61800
Thousand Young Talents Program of China

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