Tuning the Properties of Halide Nanocomposite Solid Electrolytes with Diverse Oxides for All-Solid-State Batteries

Abstract

Herein, we report halide nanocomposite solid electrolytes (HNSEs) that integrate diverse oxides with alterations that allow tuning of their ionic conductivity, (electro)chemical stability, and specific density. A two-step mechanochemical process enabled the synthesis of multimetal (or nonmetal) HNSEs, MO2-2Li(2)ZrCl(6), as verified by pair distribution function and X-ray diffraction analyses. The multimetal (or nonmetal) HNSE strategy increases the ionic conductivity of Li2ZrCl6 from 0.40 to 0.82 mS cm(-1). Additionally, cyclic voltammetry test findings corroborated the enhanced passivating properties of the HNSEs. Notably, incorporating SiO2 into HNSEs leads to a substantial reduction in the specific density of HNSEs, demonstrating their strong potential for achieving a high energy density and lowering costs. Fluorinated SiO2-2Li(2)ZrCl(5)F HNSEs exhibited enhanced interfacial compatibility with Li6PS5Cl and LiCoO2 electrodes. Cells employing SiO2-2Li(2)ZrCl(5)F with LiCoO2 exhibit superior electrochemical performance delivering the initial discharge capacity of 162 mA h g(-1) with 93.7% capacity retention at the 100th cycle at 60 degrees C.