Graphical Abstract
![](https://wqketang.oss-cn-beijing.aliyuncs.com/zip-unzip/zip-d4b01a55-7982-41de-8fed-2eea429fa941/EMD-2023-0020/files/EMD-2023-0020-revise-final-Abstract.jpg?Expires=1725755628&OSSAccessKeyId=STS.NT5eViCkqzTYdbfdqxMkjpyyq&Signature=gdarhGCbbHr0%2Ftc8oWawH3tC2p0%3D&security-token=CAISywJ1q6Ft5B2yfSjIr5eALuzdrrRQzZayZkTXgHEtQeRGn7zSkzz2IHtKenhsBOsbtfk1mG5W5%2FgZlqJ9SptIAEfJa9d99MzUP%2FpFltCT1fau5Jko1beHewHKeTOZsebWZ%2BLmNqC%2FHt6md1HDkAJq3LL%2Bbk%2FMdle5MJqP%2B%2FUFB5ZtKWveVzddA8pMLQZPsdITMWCrVcygKRn3mGHdfiEK00he8TouufTinpHMskGA1Aell7Mvyt6vcsT%2BXa5FJ4xiVtq55utye5fa3TRYgxowr%2Fwo0v0YpGya5YzHXwcPskvdKZbo78UqLQlla6w%2BGqFJqvPxr%2Fp8t%2Fx5fWJKAezhVgs8cVM8JOjIqKOscIsiJsO71SmqFV55c8Fdm%2BgUooJVgIMhTnduUfAPJAGOxzJitP%2BUVGGphr60TEnBL4rB5MUctfzRp75SXVPUTzDnGoABjuNLcf76FQN6p3t%2BSlCg%2FxR5C72RIk78k%2BUi44L9ZBmFT6F8GV7aXA52D1Ps56knKF6PAnhRivwyTxgsolycBfvccb3t5jGJ24SgY0aYosAECutxAo7sJhSwlwZvGwGDZJsop1vGiZ8eN1MbtZeRRuMeaZ2I%2BQo%2BnVP6Cf%2F0pDsgAA%3D%3D)
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Van der Waals heterostructures made up of different two-dimensional (2D) materials have garnered considerable attention as anodes for lithium-ion batteries (LIBs), and doping can significantly influence their electronic structures and lithium diffusion barriers. In this work, the effects of heteroatom (X = N, O, P, and S) doping in the graphene of the graphene/silicene (G/Si) heterostructure are comprehensively examined by using first-principles calculations. The stacking stability and mechanical stiffness of G/Si and doped G/Si (XG/Si) exhibit that N-doping can improve the structural stability of G/Si, thereby ensuring good cycling performance. The densities of states reveal that the dopants (N, O, and S) can greatly increase the electronic conductivity of G/Si. Importantly, the adsorption and diffusion behaviors of Li are primarily affected by the dopant and the doping site, resulting in ultrafast Li diffusivity. Therefore, N-doped G/Si at doping site 1 (S1) shows a good and balanced property, which exhibits high potential to enhance the electrical performance of G/Si materials and offers a reference for selecting dopants in other 2D anode materials for LIBs.
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