The increasing demands for high-performance energy storage devices have driven to develop advanced lithium batteries. However, the dendrite growth with potential safety issues greatly restricted the practical applications. Herein, the iron nitride (Fe2N) nanoparticles were anchored on carbon cloth to regulate the surface lithiophilic properties based on the theoretical prediction and experimental examination. Typically, the in-situ formation of highly porous Fe2N coating layer bridging between carbon cloth and lithium is able to regulate the interface properties of three-dimensional composite electrodes for reversible deposition and stripping of Li. The theoretical calculation revealed that Fe2N nanoparticles as lithiophilic sites would induce the uniform Li deposition due to the favorable electron transfer. Therefore, the composite Li electrode exhibited a good long-cycling performance of 1000 h in symmetric cells. When paired with LiNi0.5Co0.2Mn0.3O2 (NCM 523) and 3DC@I2 cathodes, the full cells delivered reversible capacities of 110 mAh g−1 for 200 cycles, and 140 mAh g−1 after 5000 cycles, respectively. This work gains the new insights into the efficient regulation of interface properties via the metal nitride coating to stabilize the lithium metal anode with enhanced reversibility.
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