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

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.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [4];  [5];  [5];  [6]; ORCiD logo [6];  [6];  [2]; ORCiD logo [5];  [4]; ORCiD logo [2]
  1. Harbin Inst. of Technology (China). MIIT Key Lab. of Critical Materials Technology for New Energy Conversion and Storage; Columbia Univ., New York, NY (United States)
  2. Harbin Inst. of Technology (China). MIIT Key Lab. of Critical Materials Technology for New Energy Conversion and Storage
  3. Harbin Inst. of Technology (China). MIIT Key Lab. of Critical Materials Technology for New Energy Conversion and Storage; Univ. of Western Ontario, London, ON (Canada)
  4. Univ. of Western Ontario, London, ON (Canada)
  5. Columbia Univ., New York, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1716781
Report Number(s):
BNL-220625-2020-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; U1932205; 2190507; 2017KJHZ002
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Batteries

Citation Formats

Lou, Shuaifeng, Liu, Qianwen, Zhang, Fang, Liu, Qingsong, Yu, Zhenjiang, Mu, Tiansheng, Zhao, Yang, Borovilas, James, Chen, Yijun, Ge, Mingyuan, Xiao, Xianghui, Lee, Wah-Keat, Yin, Geping, Yang, Yuan, Sun, Xueliang, and Wang, Jiajun. Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries. United States: N. p., 2020. Web. doi:10.1038/s41467-020-19528-9.
Lou, Shuaifeng, Liu, Qianwen, Zhang, Fang, Liu, Qingsong, Yu, Zhenjiang, Mu, Tiansheng, Zhao, Yang, Borovilas, James, Chen, Yijun, Ge, Mingyuan, Xiao, Xianghui, Lee, Wah-Keat, Yin, Geping, Yang, Yuan, Sun, Xueliang, & Wang, Jiajun. Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries. United States. https://doi.org/10.1038/s41467-020-19528-9
Lou, Shuaifeng, Liu, Qianwen, Zhang, Fang, Liu, Qingsong, Yu, Zhenjiang, Mu, Tiansheng, Zhao, Yang, Borovilas, James, Chen, Yijun, Ge, Mingyuan, Xiao, Xianghui, Lee, Wah-Keat, Yin, Geping, Yang, Yuan, Sun, Xueliang, and Wang, Jiajun. Wed . "Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries". United States. https://doi.org/10.1038/s41467-020-19528-9. https://www.osti.gov/servlets/purl/1716781.
@article{osti_1716781,
title = {Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries},
author = {Lou, Shuaifeng and Liu, Qianwen and Zhang, Fang and Liu, Qingsong and Yu, Zhenjiang and Mu, Tiansheng and Zhao, Yang and Borovilas, James and Chen, Yijun and Ge, Mingyuan and Xiao, Xianghui and Lee, Wah-Keat and Yin, Geping and Yang, Yuan and Sun, Xueliang and Wang, Jiajun},
abstractNote = {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.},
doi = {10.1038/s41467-020-19528-9},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Wed Nov 11 00:00:00 EST 2020},
month = {Wed Nov 11 00:00:00 EST 2020}
}