Revealing the Role of Liquid Metals at the Anode-Electrolyte Interface for All Solid-State Lithium-Ion Batteries

All-solid-state lithium-ion batteries (ASSLIBs) are receiving tremendous attention for safety concerns over liquid system. However, current ASSLIBs still suffer from poor cycling and rate performance because of unfavorable interfacial contact between solid electrolyte and electrodes, especially in the alloy-based anode. To wet the solid electrode/electrolyte interface, accommodate volume change, and further boost kinetics, liquid metal Ga is introduced into the representative Sb anode, and its corresponding role is comprehensively revealed by experimental results and theoretical calculations for the first time. In addition to interface contact and strain accommodation, with the aid of in situ generation of liquid metal Ga, the lithiation/de-lithiation activity of Sb is stimulated, showing outstanding rate and cycling performance in half cells. Furthermore, benefited from the in situ chemical reaction, TiS₂ powder can be directly used to construct a novel "Li-free" TiS₂|LiBH₄|GaSb full cell, which exhibits an outstanding capacity retention of 226 mA h g^-1 after 1000 cycles at a current density of 0.5 A g^-1. This work provides guidance for implementing future rational design of alloy anodes within ASSLIBs.