Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries

Abstract Solid polymer electrolytes with large-scale processability and interfacial compatibility are promising candidates for solid-state lithium metal batteries. Among various systems, poly(vinylidene fluoride)-based polymer electrolytes with residual solvent are appealing for room-temperature battery operations. However, their porous structure and limited ionic conductivity hinder practical application. Herein, we propose a phase regulation strategy to disrupt the symmetry of poly(vinylidene fluoride) chains and obtain the dense composite electrolyte through the incorporation of MoSe 2 sheets. The electrolyte with high dielectric constant can optimize the solvation structures to achieve high ionic conductivity and low activation energy. The in-situ reactions between MoSe 2 and Li metal generate Li 2 Se fast conductor in solid electrolyte interphase, which improves the Coulombic efficiency and interfacial kinetics. The solid-state Li||Li cells achieve robust cycling at 1 mA cm −2 , and the Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells show practical performance at high rate (3C), high loading (2.6 mAh cm −2 ) and in pouch cell.