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

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 10C. Additionally, in a full‐cell configuration with LiFePO4, 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.