Selectively Wetted Rigid–Flexible Coupling Polymer Electrolyte Enabling Superior Stability and Compatibility of High-Voltage Lithium Metal Batteries

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

doi:10.1002/aenm.201903939

Selectively Wetted Rigid–Flexible Coupling Polymer Electrolyte Enabling Superior Stability and Compatibility of High-Voltage Lithium Metal Batteries

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

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

161 Scopus citations

Abstract

Solid polymer electrolytes (SPEs) are considered to be the key to solve the safety hazards and cycling performance of liquid high-voltage lithium metal batteries (HVLMBs), but still suffer from low conductivity and poor interfacial compatibility. Here, polyvinylidene fluoride–polyvinyl acetate-based (PVDF–PVAC) rigid–flexible coupling SPE selectively wetted by a tetramethylene sulfone (TMS) is prepared for high-performance and superior-safety HVLMBs. The intermolecular interactions in such SPE significantly facilitate lithium-ion conductivity and electrolyte/electrode interface wettability. Moreover, PVAC selectively wetted with the TMS enhances interface compatibility with Li anodes and high-voltage LiCoO₂ cathodes. As a result, the as-assembled LiCoO₂/lithium-metal solid-state batteries present excellent cyclability with 85% capacity retention after 200 cycles between 3.0 and 4.5 V at room temperature. Furthermore, pouch cells with the as-prepared SPE exhibit brilliant safety and superior interfacial compatibility. This study offers a promising and general selectively wetted design strategy to handle the compatibility and safety issues in HVLMBs.

Original language	English
Article number	1903939
Journal	Advanced Energy Materials
Volume	10
Issue number	18
DOIs	https://doi.org/10.1002/aenm.201903939
State	Published - 1 May 2020
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Funding

X.Y. and L.W. contributed equally to this work. This work was supported by the National Key R&D Program of China (2018YFB0104300), the National Natural Science Foundation of China (No. 21975274), 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, P. R. China (2018GGX104016), and the National Natural Science Foundation of China (U1706229), supported by QIBEBT (ZZBS201808).

Funders	Funder number
National Key R&D Program of China	2018YFB0104300
QIBEBT	ZZBS201808
Key Technology Research and Development Program of Shandong	U1706229, 2018GGX104016
National Natural Science Foundation of China	21975274
Chinese Academy of Sciences	XDA22010600
Youth Innovation Promotion Association	2016193
National Science Fund for Distinguished Young Scholars	51625204

Keywords

high voltage
interfacial compatibility
lithium metal batteries
polymer electrolytes
safety and stability

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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abstract = "Solid polymer electrolytes (SPEs) are considered to be the key to solve the safety hazards and cycling performance of liquid high-voltage lithium metal batteries (HVLMBs), but still suffer from low conductivity and poor interfacial compatibility. Here, polyvinylidene fluoride–polyvinyl acetate-based (PVDF–PVAC) rigid–flexible coupling SPE selectively wetted by a tetramethylene sulfone (TMS) is prepared for high-performance and superior-safety HVLMBs. The intermolecular interactions in such SPE significantly facilitate lithium-ion conductivity and electrolyte/electrode interface wettability. Moreover, PVAC selectively wetted with the TMS enhances interface compatibility with Li anodes and high-voltage LiCoO2 cathodes. As a result, the as-assembled LiCoO2/lithium-metal solid-state batteries present excellent cyclability with 85% capacity retention after 200 cycles between 3.0 and 4.5 V at room temperature. Furthermore, pouch cells with the as-prepared SPE exhibit brilliant safety and superior interfacial compatibility. This study offers a promising and general selectively wetted design strategy to handle the compatibility and safety issues in HVLMBs.",

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AB - Solid polymer electrolytes (SPEs) are considered to be the key to solve the safety hazards and cycling performance of liquid high-voltage lithium metal batteries (HVLMBs), but still suffer from low conductivity and poor interfacial compatibility. Here, polyvinylidene fluoride–polyvinyl acetate-based (PVDF–PVAC) rigid–flexible coupling SPE selectively wetted by a tetramethylene sulfone (TMS) is prepared for high-performance and superior-safety HVLMBs. The intermolecular interactions in such SPE significantly facilitate lithium-ion conductivity and electrolyte/electrode interface wettability. Moreover, PVAC selectively wetted with the TMS enhances interface compatibility with Li anodes and high-voltage LiCoO2 cathodes. As a result, the as-assembled LiCoO2/lithium-metal solid-state batteries present excellent cyclability with 85% capacity retention after 200 cycles between 3.0 and 4.5 V at room temperature. Furthermore, pouch cells with the as-prepared SPE exhibit brilliant safety and superior interfacial compatibility. This study offers a promising and general selectively wetted design strategy to handle the compatibility and safety issues in HVLMBs.

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Selectively Wetted Rigid–Flexible Coupling Polymer Electrolyte Enabling Superior Stability and Compatibility of High-Voltage Lithium Metal Batteries

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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