Preparation and Characterization of Silica-Based Ionogel Electrolytes and Their Application in Solid-State Lithium Batteries

In this study, tetraethyl orthosilicate (TEOS) and methyltriethoxysilane (MTES) were used as precursors for silica, combined with the ionic liquid [BMIM-ClO4]. Lithium perchlorate was added as the lithium-ion source, and formic acid was employed as a catalyst to synthesize silica ionogel electrolytes via the sol-gel method. FT-IR and NMR identified the self-prepared ionic liquid [BMIM-ClO4], and its electrochemical window was determined using linear sweep voltammetry (LSV). The properties of the prepared silica ionogel electrolytes were further investigated through FT-IR, DSC, and 29Si MAS NMR measurements, followed by electrochemical property measurements, including conductivity, electrochemical impedance spectroscopy (EIS), LSV, and charge-discharge tests. The experimental results showed that adding methyltriethoxysilane (MTES) enhanced the mechanical strength of the silica ionogel electrolyte, simplifying its preparation process. The prepared silica ionogel electrolyte exhibited a high ionic conductivity of 1.65 × 10-3 S/cm. In the LSV test, the silica ionogel electrolyte demonstrated high electrochemical stability, withstanding over 5 V without oxidative decomposition. Finally, during the discharge-charge test, the second-cycle capacity reached 108.7 mAh/g at a discharge-charge rate of 0.2 C and a temperature of 55 °C.