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

• Published in: Frontiers of materials science Vol. 18; no. 2
• Main Authors: Liang, Xinghua, Shen, Pengcheng, Lan, Lingxiao, Qin, Yunmei, Yan, Ge, Huang, Meihong, Lu, Xuanan, Hun, Qiankun, Wang, Yujiang, Wang, Jixuan
• Format: Journal Article
• Language: English
• Published: Beijing Higher Education Press 01.06.2024; Springer Nature B.V
• Subjects: Chemistry and Materials Science; Curing; Electrolytes; Ion currents; Lithium; Lithium batteries; Lithium ions; Materials Science; Molten salt electrolytes; Polymethyl methacrylate; Research Article; Room temperature; Solid electrolytes; Solid state; Stability; Tensile strength; Vinylidene; Vinylidene fluoride; lithium-ion transference number; electrochemical reliability; lithium metal battery; double-layer solid composite electrolyte
• ISSN: 2095-025X; 2095-0268
• DOI: 10.1007/s11706-024-0685-9

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 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (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.