The ability of Al- and Ga-doped graphene (Al-Gr/Ga-Gr) to activate the C‒H bond of CH4 by N2O and methanol production is investigated using density functional theory calculations. Both surfaces have a higher affinity for capturing N2O than CH4. The oxidation of CH4 starts with the decomposition of N2O into N2 and Oads species, followed by a hydrogen transfer from CH4 to Oads, resulting in CH3 and HOads species. Our results demonstrate that the CH3 combination with HOads to yield CH3OH needs only 0.18 eV on Al-Gr, which is lower than on Ga-Gr. The competing CO oxidation reaction (CO + Oads → CO2), on the other hand, is inhibited on the Ga-Gr because to its greater activation barrier than the CH4 oxidation process. These findings may provide valuable information for fine-tuning the catalytic activity of graphene-based materials in low-temperature partial oxidation of CH4.
