Mixed Ion/Electron Conductive Li₃N–Mo Interphase Enabling Stable and Ultrahigh-Rate Lithium Metal Anodes

Lithium (Li) metal is a promising anode for high-energy-density batteries; however, its practical viability is hampered by the unstable metal Li–electrolyte interface and Li dendrite growth. Herein, a mixed ion/electron conductive Li 3 N–Mo protective interphase with high mechanical stability is designed and demonstrated to stabilize the Li–electrolyte interface for a dendrite-free and ultrahigh-current-density metallic Li anode. The Li 3 N–Mo interphase is simultaneously formed and homogeneously distributed on the Li metal surface by the surface reaction between molten Li and MoN nanosheets powder. The highly ion-conductive Li 3 N and abundant Li 3 N/Mo grain boundaries facilitate fast Li-ion diffusion, while the electrochemically inert metal Mo cluster in the mosaic structure of Li 3 N–Mo inhibits the long-range crystallinity and regulates the Li-ion flux, further promoting the rate capability of the Li anode. The Li 3 N–Mo/Li electrode has a stable Li–electrolyte interface as manifested by a low Li overpotential of 12 mV and outstanding plating/stripping cyclability for over 3200 h at 1 mA cm –2 . Moreover, the Li 3 N–Mo/Li anode inhibits Li dendrite formation and exhibits a long cycling life of 840 h even at 30 mA cm –2 . The full cell assembled with LiFePO 4 cathode exhibits stable cycling performance with 87.9% capacity retention for 200 cycles at 1C (1C = 170 mA g –1 ) as well as high rate capability of 83.7 mAh g –1 at 3C. The concept of constructing a mixed ion/electron conductive interphase to stabilize the Li–electrolyte interface for high-rate and dendrite-free Li metal anodes offers a viable strategy to develop high-performance Li-metal batteries.