High-stability double-layer polymer‒inorganic composite electrolyte fabricated through ultraviolet curing process for solid-state lithium metal batteries

Abstract

Electrolyte interface resistance and low ionic conductivity are essential issues for commercializing solid-state lithium metal batteries (SSLMBs). This work details the fabrication of a double-layer solid composite electrolyte (DLSCE) for SSLMBs. The composite comprises poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF‒HFP) and poly(methyl methacrylate) (PMMA) combined with 10 wt.% of Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO), synthesized through an ultraviolet curing process. The ionic conductivity of the DLSCE (2.6 × 10⁻⁴ S·cm⁻¹) at room temperature is the high lithium-ion transference number (0.57), and the tensile strength is 17.8 MPa. When this DLSCE was assembled, the resulted LFP/DLSCE/Li battery exhibited excellent rate performance, with the discharge specific capacities of 162.4, 146.9, 93.6, and 64.0 mA·h·g⁻¹ at 0.1, 0.2, 0.5, and 1 C, respectively. Furthermore, the DLSCE demonstrates remarkable stability with lithium metal batteries, facilitating the stable operation of a Li/Li symmetric battery for over 200 h at both 0.1 and 0.2 mA·cm⁻². Notably, the formation of lithium dendrites is also effectively inhibited during cycling. This work provides a novel design strategy and preparation method for solid composite electrolytes.

Keywords

electrochemical reliability / lithium metal battery / lithium-ion transference number / double-layer solid composite electrolyte

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Authors’ contributions

Conceptualization, X.L. and P.S.; methodology, J.W.; software, P.S.; validation, X.L., P.S. and G.Y.; formal analysis, M.H. and Y.W.; investigation, P.S. and Q.H; resources, X.L.; data curation, P.S.; writing — original draft preparation, P.S.; writing — review and editing, X.L.; visualization, L.L.; supervision, X.L.; project administration, X.L.; funding acquisition, L.L. All authors have read and agreed to the published version of the manuscript.

Declaration of competing interests

The authors declare that they have no competing interests.

Acknowledgements

This research was supported by the Liuzhou Science and Technology Fund Project (Grant No. 2023PRj0103), the National Natural Science Foundation of China (Grant Nos. 52161033 and 22262005), the Guangxi Key Laboratory of Automobile Components and Vehicle Technology Fund Project (Grant Nos. 2022GKLACVTKF02 and 2023GKLACVTZZ02), and the Fund Project of the Key Lab of Guangdong Science and Technology Innovation Strategy Special Fund Project in 2023 (Grant No. pdjh2023a0819).

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