Controlling electronic properties of MoS₂/graphene oxide heterojunctions for enhancing photocatalytic performance: the role of oxygen

Abstract

The manipulation of the constituents of novel hetero-photocatalysts is an effective method for improving photocatalytic efficiency, but a theoretical understanding of the relationship between interlayer interaction and photocatalytic activity is still lacking. Herein, the interfacial interactions and electronic properties of MoS₂/graphene oxide (GO) heterojunctions with various O concentrations were explored systematically by first-principles calculations. The results indicate that MoS₂ and GO can form a stable van der Waals heterojunction, and enhance the built-in internal electric field from GO to the MoS₂ surface with the increase in O concentration after interfacial equilibrium. It is inferred that the photogenerated electrons and holes naturally accumulate in the conduction band of GO and the valence band of MoS₂, respectively, under the built-in internal electric field driving, indicating the formation of direct Z-scheme heterojunctions. In addition, a red shift of the light absorption edge and the shift up of the conduction band edge of MoS₂/GO heterojunctions are observed with an increase in O concentration. It can be concluded that the O atom plays a crucial role in the energy band alignment of MoS₂/GO heterojunctions for the improvement of photocatalytic performance. These results are beneficial to understand and design layered MoS₂/GO photocatalytic systems or as cocatalysts with other semiconductors.