Understanding the Coupling Mechanism of Intercalation and Conversion Hybrid Storage in Lithium–Graphite Anode

Abstract Anodes with high capacity and long lifespan play an important role in the advanced batteries. However, none of the existing anodes can meet these two requirements simultaneously. Lithium (Li)–graphite composite anode presents great potential in balancing these two requirements. Herein, the working mechanism of Li–graphite composite anode is comprehensively investigated. The capacity decay features of the composite anode are different from those of Li ion intercalation in Li ion batteries and Li metal deposition in Li metal batteries. An intercalation and conversion hybrid storage mechanism are proposed by analyzing the capacity decay ratios in the composite anode with different initial specific capacities. The capacity decay models can be divided into four stages including Capacity Retention Stage, Relatively Independent Operation Stage, Intercalation & Conversion Coupling Stage, Pure Li Intercalation Stage. When the specific capacity is between 340 and 450 mAh g −1 , its capacity decay ratio is between that of pure intercalation and conversion model. These results intensify the comprehensive understandings on the working principles in Li–graphite composite anode and present novel insights in the design of high‐capacity and long‐lifespan anode materials for the next‐generation batteries.