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Research Article

An artificial interphase enables stable PVDF-based solid-state Li metal batteries

Mengjun Wu1,§, Jiangping Song1,§, Jiaheng Lei2, Haolin Tang1,3( )
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Department of Chemistry, School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China
Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan 528200, China

§ Mengjun Wu and Jiangping Song contributed equally to this work.

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Graphical Abstract

A K+ added polymer interlayer by ultraviolet (UV) polymerization of poly(ethylene glycol) methyl ether methacrylate (PEGMA)-based precursor solution is coated on the Li surface to enhance the interfacial stability between polyvinylidene fluoride (PVDF)-based composite polymer electrolyte (CPE) and Li anode. The PVDF electrolytes united with this PEG-KNO3 layer enable the Li|LFP (LFP = LiFePO4) cell with high loading of 10 mg·cm−2 to cycle over 60 cycles without significant capacity loss.

Abstract

Composite polymer electrolytes (CPEs) have attracted much attention for high energy density solid-state lithium-metal batteries owing to their flexibility, low cost, and easy scale-up. However, the unstable Li/CPE interface is always challengeable for the practical utilization of CPEs. Herein, a polymer interlayer containing K+ prepared by ultraviolet (UV)-curing precursor solution is coated on Li surface to stabilize the interface between poly(vinylidene difluoride) (PVDF) composite electrolytes and Li anode. Benefiting from the physical barrier of the interlayer, the continuous decomposition of PVDF is restrained and the intimate contact between electrode and electrolyte is also achieved to reduce the interface impedance. Moreover, the added K+ is utilized to further regulate smooth Li deposition. As a consequence, the symmetric Li|Li cell with coated Li demonstrates steady cycling at 0.4 mAh·cm−2 and a high critical current density of 1 mA·cm−2. The assembled Li|LiFePO4 cell presents outstanding cycling stability (capacity retention of 90% after 400 cycles at 1 C) and good rate performance. The associated pouch cell performs impressive flexibility and safety. This work provides a convenient strategy to achieve stable Li/PVDF interface for high-performance PVDF-based solid state Li metal batteries.

Keywords

interfacial modificationsolid-state batteriescomposite polymer electrolytesinterfacial compatibilitylithium dendrite

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Nano Research
Volume 17 Issue 3,
March 2024
Pages 1482-1490
DOI: 10.1007/s12274-023-5963-9
Cite this article:
Wu M, Song J, Lei J, et al. An artificial interphase enables stable PVDF-based solid-state Li metal batteries. Nano Research, 2024, 17(3): 1482-1490. https://doi.org/10.1007/s12274-023-5963-9
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Received: 10 May 2023
Revised: 22 June 2023
Accepted: 26 June 2023
Published: 27 July 2023
© Tsinghua University Press 2023
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