Complementary modulation of Li adsorption and diffusion kinetics in B-, N-, and noble-metal-co-doped γ-graphyne for...

Heteroatom doping offers an effective strategy to tailor the properties of carbon-based anode materials for lithium-ion batteries (LIBs). Building on our recent study of noble metal-doped γ-graphyne (γ-GY), we herein employ dispersion-corrected density functional theory to investigate a co-doping strategy incorporating non-metal atoms (B, N) with these noble metals. The resulting B-M-γ-GY, N-M-γ-GY and B-M-N-γ-GY configurations all exhibit excellent structural integrity and robust thermal stability. Importantly, co-doping effectively modulates the electronic structure, yielding metallic or near-metallic behavior favorable for electron transport. Meanwhile, B-M-N-γ-GY systems maintain high Li adsorption energies, which prevent Li clustering, and deliver theoretical specific capacities exceeding 1000 mAh g^-1. Notably, along the selected H → H₁ migration pathway, the B-Pt-N-γ-GY and B-Ru-N-γ-GY systems exhibit low Li diffusion barriers of 0.66 and 0.67 eV, respectively, with corresponding diffusion coefficients that are several orders of magnitude higher than that of pristine γ-GY. This work establishes that strategic co-doping of non-metal and noble metal atoms in γ-GY offers an effective pathway for balancing and optimizing the key kinetic and thermodynamic properties for high-performance LIB anodes.