Multi‐Dimensional Interphase Modulation by Plasma for Construction of Advanced Lithium Metal Batteries

Abstract Reaction interphase modulation plays a key role in the performance of lithium metal anodes. Herein, novel hybrid plasma technologies are developed to regulate three main interfaces including the bottom nucleation interface between the backbone and lithium, the middle interface between solid electrolyte interphase (SEI) and lithium, and the upper interface between SEI and electrolyte to achieve uniform deposition of Li + and suppress the growth of dendrite. Specifically, plasma‐derived vertical graphene is grown on sponge nickel fiber to optimize the bottom nucleation interface, which can spontaneously form a gradient distribution of current density to induce a uniform bottom‐to‐up deposition of Li. On this base, a unique tri‐gradient inorganic‐organic SEI (Li 3 N/Li 2 O─RCOOLi) is constructed on Li metal via N 2 and ethylene carbonate hybrid plasma. The plasma‐SEI is dominated by inorganic components, where the outer layer is Li 3 N/Li 2 O‐rich interphase with a low desolvation energy for electrolyte and the inner layer is mainly composed of Li 2 O with a high interfacial energy to promote a lateral diffusion of Li. The designed interphases synergistically enhance the structure and interface stability, reduce side reactions with electrolyte, facilitate uniform deposition of lithium, and suppress the Li dendrite, leading to an enhanced cycling life of 2275 h and high coulombic efficiency.