van der Waals heterostructure for photocatalysis: Graphitic carbon nitride and Janus transition-metal dichalcogenides

Abstract: Converting solar energy into chemical energy by splitting water is a promising means to generate a sustainable and renewable solution without detrimental environmental impact. The two-dimensional semiconductors serve as potential catalysts in this regard, and here we combine Janus transition-metal dichalcogenides (MoXY, X/Y = S, Se, Te) and graphitic carbon nitride in a van der Waals heterostructure. Within the first-principles calculations, we investigate the electronic, optical and excitonic properties that determine the photocatalytic activity. Due to the internal electric field, the photogenerated electrons and holes are separated in the MoXY layers, and also generates high overpotentials for the redox reactions. The high optical absorptions span throughout the entire visible and near ultraviolet regime in these heterostructure nanocomposites. Further, the lower exciton binding, calculated within the two-dimensional hydrogenic model, indicates efficient charge separation. Enormous tunability of photocatalytic properties in such heterostructures should attract considerable theoretical and experimental attention in future.