A Bifunctional Chemomechanics Strategy to Suppress Electrochemo-Mechanical Failure of Ni-Rich Cathodes for All-Solid-State Lithium Batteries

Xingwei Sun; Longlong Wang; Jun Ma; Xinrun Yu; Shu Zhang; Xinhong Zhou; Guanglei Cui

doi:10.1021/acsami.2c02678

A Bifunctional Chemomechanics Strategy to Suppress Electrochemo-Mechanical Failure of Ni-Rich Cathodes for All-Solid-State Lithium Batteries

Xingwei Sun, Longlong Wang, Jun Ma, Xinrun Yu, Shu Zhang, Xinhong Zhou, Guanglei Cui

Research output: Contribution to journal › Article › peer-review

34 Scopus citations

Abstract

Electrochemo-mechanical failure of Ni-rich cathodes leads to rapid performance degradation, and thus hinders their practical implementation in all-solid-state lithium batteries (ASSLBs). To solve this problem, herein, we propose a bifunctional chemomechanics strategy by protecting polycrystalline LiNi_0.6Co_0.2Mn_0.2O₂(NCM) cathodes using a high-mechanical-strength fast ionic conductor LiZr₂(PO₄)₃(LZP) coating layer. The coating layer's synergistic effect between mechanical strength and electrochemical stability is studied in Li₆PS₅Cl (LPSCl)-based ASSLBs for the first time. Using finite element method (FEM) simulations and various characterization techniques, we demonstrate that the robust and stable LZP (Young's modulus 140.7 GPa, electrochemical stability window >5 V) coating layer mitigates the volume change and particle disintegration of polycrystalline NCM and electrochemical decomposition of LPSCl on the LPSCl/NCM interface. As a result, the LZP-modified ASSLBs display remarkably improved reversible capacity, cycle life, and rate performance. The synergy of mechanical and electrochemical properties of the coating layer will provide valuable guidance for the development of high-energy-density ASSLBs.

Original language	English
Pages (from-to)	17674-17681
Number of pages	8
Journal	ACS Applied Materials and Interfaces
Volume	14
Issue number	15
DOIs	https://doi.org/10.1021/acsami.2c02678
State	Published - 20 Apr 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

Funding

This work was supported by the Key Area Research and Development Program of Guangdong Province (2020B090919005), the National Natural Science Foundation of China (21975274), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA22010600), Shandong Provincial Natural Science Foundation (ZR2020KE032), the Youth Innovation Promotion Association of CAS (2021210), and the Shandong Energy Institute (SEI) (SEII202117). The authors gratefully acknowledge Prof. Kejie Zhao (School of Mechanical Engineering at Purdue University) for the valuable discussions and kind help on FEM simulations.

Funders	Funder number
Shandong Energy Institute	SEII202117
National Natural Science Foundation of China	21975274
Chinese Academy of Sciences	XDA22010600
Youth Innovation Promotion Association of the Chinese Academy of Sciences	2021210
Natural Science Foundation of Shandong Province	ZR2020KE032
Special Project for Research and Development in Key areas of Guangdong Province	2020B090919005

Keywords

Ni-rich all-solid-state lithium battery
bifunctional chemomechanics strategy
electrochemical stability
electrochemo-mechanical failure
high mechanical strength

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10.1021/acsami.2c02678

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title = "A Bifunctional Chemomechanics Strategy to Suppress Electrochemo-Mechanical Failure of Ni-Rich Cathodes for All-Solid-State Lithium Batteries",

abstract = "Electrochemo-mechanical failure of Ni-rich cathodes leads to rapid performance degradation, and thus hinders their practical implementation in all-solid-state lithium batteries (ASSLBs). To solve this problem, herein, we propose a bifunctional chemomechanics strategy by protecting polycrystalline LiNi0.6Co0.2Mn0.2O2(NCM) cathodes using a high-mechanical-strength fast ionic conductor LiZr2(PO4)3(LZP) coating layer. The coating layer's synergistic effect between mechanical strength and electrochemical stability is studied in Li6PS5Cl (LPSCl)-based ASSLBs for the first time. Using finite element method (FEM) simulations and various characterization techniques, we demonstrate that the robust and stable LZP (Young's modulus 140.7 GPa, electrochemical stability window >5 V) coating layer mitigates the volume change and particle disintegration of polycrystalline NCM and electrochemical decomposition of LPSCl on the LPSCl/NCM interface. As a result, the LZP-modified ASSLBs display remarkably improved reversible capacity, cycle life, and rate performance. The synergy of mechanical and electrochemical properties of the coating layer will provide valuable guidance for the development of high-energy-density ASSLBs.",

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A Bifunctional Chemomechanics Strategy to Suppress Electrochemo-Mechanical Failure of Ni-Rich Cathodes for All-Solid-State Lithium Batteries

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