Lithiophilic Zn3N2-Modified Cu Current Collectors by a Novel FCVA Technology for Stable Anode-Free Lithium Metal Batteries.

Abstract

Anode-free lithium metal batteries (AFLMBs) offer high-energy-density battery systems, but their commercial viability is hindered by irregular lithium dendrite growth and "dead Li" formation caused by current collector defects. This study employed filtered cathode vacuum arc (FCVA) technology to fabricate Cu current collectors (CCs) with a lithiophilic Zn3N2 film. This advanced preparation process ensures an evenly distributed film that reduces the nucleation overpotential, homogenizes the interfacial electric field during plating/stripping processes, inhibits lithium dendrite growth, and forms a stable solid-electrolyte interphase (SEI). Our results show that the advanced Zn3N2@Cu CCs exhibit superior performance with a high CE of above 99.3% after 230 cycles at a current density of 0.5 mA cm-2 and an area capacity of 1 mAh cm-2. Additionally, Li-Zn3N2@Cu||Li-Zn3N2@Cu symmetrical cells had a longer stable cycle time of over 1000 h than that of Li||Li and Li-Cu||Li-Cu symmetrical cells at a current density of 1 mA cm-2 and an area capacity of 2 mAh cm-2. Compared with bare Cu CCs, the capacity retention rate is increased from 14.9 to 63.1% after 100 cycles with a 0.5C rate in the AFLMBs with LFP as the cathode. This work provides a pioneering, eco-friendly, and effective solution for the fabrication of anode CCs in AFLMBs, addressing a significant challenge in their commercial application.