In situ formation of a Li3N-rich interface between lithium and argyrodite solid electrolyte enabled by nitrogen doping

Abstract

All-solid-state Li metal batteries (ASSLMBs) have been regarded as next generation batteries due to their high energy density and safety. However, the catastrophic interface between lithium metal and solid electrolytes that leads to dendrite growth and capacity fading has stemmed the commercialization of ASSLMBs. Herein, an in situ formed Li₃N-rich interface between lithium and solid-state electrolyte is introduced via doping nitrogen into the argyrodite Li₆PS₅Cl. The critical current density of the N-doped Li₆PS₅Cl electrolyte reaches as high as 1.52 mA cm⁻² at room temperature, and the symmetric cell with the solid electrolyte can deliver a steady Li plating/stripping performance over 1000 h at a high current density of 0.5 mA cm⁻². What's more, when the N-doped Li₆PS₅Cl electrolyte is applied in full cells as a Li metal anode interlayer, prominent cycling stability and rate performance can be achieved. This work provides a promising strategy to design ASSLMBs with high energy density.