Composite polymer electrolytes with ionic liquid grafted-Laponite for dendrite-free all-solid-state lithium metal batteries

Composite polymer electrolytes (CPEs) with high ionic conductivity and favorable electrolyte/electrode interfacial compatibility are promising alternatives to liquid electrolytes. However, severe parasitic reactions in the Li/electrolyte interface and the air-unstable inorganic fillers have hindered their industrial applications. Herein, surface-edge opposite charged Laponite (LAP) multilayer particles with high air stability were grafted with imidazole ionic liquid (IL-TFSI) to enhance the thermal, mechanical, and electrochemical performances of polyethylene oxide (PEO)-based CPEs. The electrostatic repulsion between multilayers of LAP-IL-TFSI enables them to be easily penetrated by PEO segments, resulting in a pronounced amorphous region in the PEO matrix. Therefore, the CPE-0.2LAP-IL-TFSI exhibits a high ionic conductivity of 1.5 × 10^-3 S cm^-1 and a high lithium-ion transference number of 0.53. Moreover, LAP-IL-TFSI ameliorates the chemistry of the solid electrolyte interphase, significantly suppressing the growth of lithium dendrites and extending the cycling life of symmetric Li cells to over 1000 h. As a result, the LiFePO₄||CPE-0.2LAP-IL-TFSI||Li cell delivers an outstanding capacity retention of 80% after 500 cycles at 2C at 60 °C. CPE-LAP-IL-TFSI also shows good compatibility with high-voltage LiNi_0.8Co_0.1Mn_0.1O₂ cathodes.