Hydrogen bond interaction derived homogeneous graphene coating on submicron silicon anode

Abstract Silicon (Si) has emerged as a promising anode material in the pursuit of higher energy‐density lithium‐ion batteries (LIBs). The large‐scale applications of Si anode, however, are hindered by its significant swelling, severe pulverization, and continuous electrode–electrolyte reaction. Therefore, the development of an efficient approach to mitigate Si particle swelling and minimize interface parasitic reactions has emerged as a prominent research focus in both academia and industry. Here, a facile and scalable strategy is reported for the preparation of a double‐layer coated submicron Si anode, comprising ceramic (silicon oxide) and graphene layers, denoted as Si@SiO x @G. In this approach, SiO x is in situ synthesized on the surface of Si and bonded with graphene through hydrogen bond interactions. The prepared Si electrode shows exceptional structural integration and demonstrates outstanding electrochemical stability, with a capacity retention of 92.58% after 540 cycles at 1 A g −1 , as well as remarkable rate capability, achieving a specific capacity of 875 mAh g −1 at 2 A g −1 . This study presents a straightforward yet pragmatic approach for the widespread implementation of high‐energy‐density silicon‐based batteries.