Carbon‐based interface engineering and architecture design for high‐performance lithium metal anodes

Abstract Metallic lithium (Li) is considered the “Holy Grail” anode material for the next‐generation of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electrochemical potential. However, owing to inhomogeneous Li‐ion flux, Li anodes undergo uncontrollable Li deposition, leading to limited power output and practical applications. Carbon materials and their composites with controllable structures and properties have received extensive attention to guide the homogeneous growth of Li to achieve high‐performance Li anodes. In this review, the correlation between the behavior of Li anode and the properties of carbon materials is proposed. Subsequently, we review emerging strategies for rationally designing high‐performance Li anodes with carbon materials, including interface engineering (stabilizing solid electrolyte interphase layer and other functionalized interfacial layer) and architecture design of host carbon (constructing three‐dimension structure, preparing hollow structure, introducing lithiophilic sites, optimizing geometric effects, and compositing with Li). Based on the insights, some prospects on critical challenges and possible future research directions in this field are concluded. It is anticipated that further innovative works on the fundamental chemistry and theoretical research of Li anodes are needed.