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Open AccessCCS ChemistryRESEARCH ARTICLES7 May 2024

A Quasi-Solid-State Electrolyte with Semi-Immobilized Solvent-Like Sites for Lithium-Metal Batteries

    https://doi.org/10.31635/ccschem.024.202404142

    Quasi solid-state lithium-metal batteries (QSSLMBs) hold significant promise for enhanced energy density when compared to conventional battery systems. Nevertheless, current QSSLMBs face challenges in lithium dendrites and electrode-electrolyte interfacial side reactions driven by excessive active free solvent molecules. Herein, a metal–organic framework (MOF) with chemically grafted soft multiether molecules (d-Gluconic acid,2,4:3,5-di-O-methylene-, denoted as G) has been proposed to serve as a solid-state electrolyte (SSE). The as-obtained M-G based electrolyte (MGE) comprises structured MOF channels with semi-immobilized solvent-like sites (G molecules), which replace liquid molecules to coordinate with Li+ ions. The MGE reduces the demand for solvents compared with traditional quasi-solid-state electrolytes, thus suppressing interface side reactions. This arrangement also facilitates achieving an elevated Li+ transference number (0.64) and a broad electrochemical stability window (5.4 V). Ultimately, the solid-state Li//Li symmetrical battery displays an extended lifetime surpassing 1500 h under 1 mA cm−2. The solid-state LiFePO4//Li battery utilizing the flame-retarded MGE attains an impressive capacity retention of 95.75% over 600 cycles. The MOF-based functionalization strategy introduces an innovative approach to designing a high-performance SSE for advanced solid-state lithium metal batteries.

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