Liquid-phase synthesis of Li_(2)S and Li_(3)PS_(4) with lithium-based organic solutions

Sulfide solid electrolytes are widely regarded as one of the most promising technical routes to realize all-solid-state batteries(ASSBs)due to their high ionic conductivity and favorable deformability.However,the relatively high price of the crucial starting material,Li_(2)S,results in high costs of sulfide solid electrolytes,limiting their practical application in ASSBs.To solve this problem,we develop a new synthesis route of Li_(2)S via liquid-phase synthesis method,employing lithium and biphenyl in 1,2-dimethoxyethane(DME)ether solvent to form a lithium solution as the lithium precursor.Because of the comparatively strong reducibility of the lithium solution,its reaction with sulfur proceeds effectively even at room temperature.This new synthesis route of Li_(2)S starts with cheap precursors of lithium,sulfur,biphenyl and DME solvent,and the only remaining byproduct(DME solution of biphenyl)after the collection of Li_(2)S product can be recycled and reused.Besides,the reaction can proceed effectively at room temperature with mild condition,reducing energy cost to a great extent.The as-synthesized Li_(2)S owns uniform and extremely small particle size,proved to be feasible in synthesizing sulfide solid electrolytes(such as the solid-state synthesis of Li_(6)PS_(5)C_(l)).Spontaneously,this lithium solution can be directly employed in the synthesis of Li_(3)PS_(4) solid electrolytes via liquid-phase synthesis method,in which the centrifugation and heat treatment processes of Li_(2)S are not necessary,providing simplified production process.The as-synthesized Li_(3)PS_(4) exhibits typical Li+conductivity of 1.85×10^(-4) S·cm^(-1) at 30℃.