Conversion of Methane to Methanol on Cobalt-Embedded Graphene: A Theoretical Perspective

Direct conversion of methane (CH 4 ) to methanol (CH 3 OH) still remains a tremendous challenge in the field of catalysis because of the high CH 3 –H bond strength. Using density functional theory calculations, we explored that Co atoms embedded in graphene (Co 1 /G) improved the catalytic performance relative to other metals embedding (Mn, Ni, W, and V) in the conversion of CH 4 . Co 1 /G showed excellent activity for the activation of C–H bond with the energy barrier of only 0.80 eV. Meanwhile, Co 1 /G exhibited remarkable selectivity for the conversion of CH 4 to CH 3 OH with the energy barrier of 0.70 eV, significantly lower than that of other by-products (1.17 eV). In addition, the existence of H 2 O molecules increased the energy barrier of the activation of C–H bond from 0.80 to 1.02 eV due to the hydrogen bond. The findings provide a new route to understanding and designing highly efficient catalysts for the direct conversion of CH 4 to CH 3 OH. Graphic Abstract