Double Carbon‐Species Coated Porous Silicon Anode Induced by Interfacial Energy Reduction for Lithium‐Ion Batteries

Abstract The rapid development of electric vehicles necessitates high‐energy density Li‐ion batteries for extended range. Silicon is a promising alternative to graphite anodes due to its high capacity; however, its substantial volume expansion during cycling leads to continuous growth of the solid electrolyte interphase and significant capacity fading. This study addresses these issues by designing a porous Si structure combined with a double carbon‐species coating layer, induced by low interfacial energy in a scalable process. Carbon and graphene are located on Si surfaces, forming a close interface that maintains electrical contact, suppresses lithium consumption, and enhances charge transfer properties. The composite anode with a double carbon‐species coating on Si demonstrates rapid stabilization with increasing coulombic efficiency, achieving a specific capacity of 1,814 mAh g −1 at 0.2 C and a high‐rate capability of 1,356 mAh g −1 at 10 C. Additionally, in a full‐cell configuration with LiFePO 4 , it recorded a specific capacity of 161 mAh g −1 at 0.2 C. These results show the potential of porous Si with a carbon‐graphene coating for stable, high‐capacity operation in Li‐ion batteries, offering new insights into high‐performance electrochemical systems. Moreover, the double carbon‐species coating derived from a scalable surface chemistry‐based process presents a realistic alternative for industrial applications.