Self‐Assembled Tent‐Like Nanocavities for Space‐Confined Stable Lithium Metal Anode

Abstract Lithium metal is considered as a promising anode for its high energy density and low redox potential. However, dendrite growth and electrolyte‐lithium reaction lead to poor cycling stability of lithium anodes. Herein, a space‐confined strategy is proposed to realize stable Li metal anode by constructing a nonplanar interface with flexible tent‐like nanocavities. The tent‐like interface is achieved through the self‐assembly of graphene oxide on zinc nanosheets, accompanied by the spontaneous formation of ZnOC bond. Remarkably, the ZnOC bond immobilizes the graphene oxide layer to ensure tent‐like structural integrity, and shows excellent lithophilicity to induce homogeneous lithium deposition within nanocavities. Furthermore, the process of Li plating/stripping is confined inside tent‐like nanocavities to effectively decrease electrolyte content contact with fresh Li, which reduces hazardous electrolyte‐lithium reaction and thus eliminates continuous consumption of Li metal. Consequently, the symmetrical cells with the tent‐like interface deliver excellent long cycling performance over 1600 h at 1 mA cm⁻², and full batteries show high‐capacity retention of 94.6% after 3000 cycles at 5 C. This strategy provides a unique flexible tent‐like interface to achieve stable lithium metal anode.