Enhanced Performance for Li & Na Ion Battery Anodes by Charge Modulation of Interface Through SiC₄ and SiN₁C₃ Active Centers on Silicon Nitrogen Co‐Doped Graphene

Abstract Heteroatom doping of graphene is a powerful approach to develop high‐performance Li and Na ion battery anodes. In this study, silicon‐nitrogen co‐doped graphene (Si−N−GN) nanostructures were successfully synthesized via a rational and scalable solvothermal process. The performances of Si−N−GN in Na + and Li + half‐cells were investigated in detail by advanced electrochemical techniques and the obtained results were analyzed in terms of Si−N−GN surface properties, reaction kinetics, and electrode/interface interactions. Si−N−GN exhibited a superior capacity of 540 mAh g −1 at a current density of 0.5 A g −1 for Li + and improved rate capability for both Li + and Na + which are linked with the increased interlayer spacing and enlarged graphene sheets upon Si‐doping. Importantly, the capacity increased with the number of cycles owing to surface electron density redistribution and Si−N−GN/SEI interactions, supported by DFT.