Superior lithium-metal all-solid-state batteries with in-situ formed Li3N-LiF-rich interphase

Lithium dendrite growth in solid electrolytes (SEs) is one of the most serious challenges to the commercialization of all-solid-state lithium-metal batteries(ASSLMBs) with SEs. Herein, we propose an electrochemical strategy to realize an in-situ modified solid electrolyte interphase (SEI) that can simultaneously resolve both interfacial and dendrite issues. By controlling the current and deposition time in electrochemical treatment, ordered reaction between lithium metal and Si3N4 particles are realized to effectively produce a Li3N-LiF-rich multifunctional composit including Li−Si alloys. The consequent symmetric cells demonstrated a remarkably high critical current density up to 3.3mA cm−2 at room temperature and stable plating/stripping process over 1200h at a current density of 0.5mA cm−2. Moreover, LiCoO2/Li6PS5Cl/Li ASSLMBs delivered a high safety and long life of more than 500 cycles at 1.0mA cm−2 with a steady coulombic efficiency.