▎ 摘　　要

Catalytic conversion of methane to commodity chemicals is highly desired. With methods of density functional theory (DFT) computations, we investigated methane conversion to methanol (MCM) with H2O2 as oxidant over Zn dimer supported by amino nitrogen and pyridinic nitrogen co-doped porous graphene (Zn2@NPG). The facile oxidation of Zn dimer gives rise to the formation of reactive site toward methane activation. The CH3-H bond cleavage with 0.24 eV energy barrier is directly followed by the formation of methanol and regeneration of Zn2@NPG. Further analysis revealed that Zn dimer is strongly stabilized and positive charged by sharing 4 s electrons with N atoms, which ensures high-stability and good electronic conductivity of the Zn2@NPG. Amino N atom exhibits efficient electronic transfer with Zn dimer by forming two Zn-N bonds, endowing its function as an electron reservoir. Amino N as an electron donator promotes oxidation of Zn dimer and as an electron acceptor facilitates deoxidation of Zn dimer and methane conversion. The combined effect of Zn dimer and amino N atoms endows Zn2@NPG with excellent electronic structure for high activity in catalyzing MCM. This work opens a new door to accomplish low-temperature methane conversion on bi-atom catalysts (BACs).