N-P Type Charge Compensatory Synergistic Effect for Schottky and Efficient Photoelectrocatalysis Applications: Doping Mechanism in (Nb/Re)@WS/Graphene Heterojunctions.

Band gap engineering based on doped two-dimensional (2D) transition metal dichalcogenides (TMDs) has shown great potential in the design and development of new nano photoelectronic devices and their application in photoelectrocatalysis. However, there are two key issues that are difficult to take into account, namely the impurity levels induced by dopant atoms appear in the forbidden band of the doping system, which can become the recombination center of photogenerated carriers, thereby reducing the photocatalytic efficiency. Compared with the carrier mobility of the corresponding doped systems, that of intrinsic 2D TMDs is too low. Understanding the doping mechanism of heteroatoms in these systems and designing corresponding crystal structures rationally is important for solving these problems. In this study, the crystal structures of co-doped monolayer WS with Nb and Re atoms were designed using density functional theory, and doping systems with graphene (high carrier mobility) were assembled into a heterostructure using the concept of heterorecombination. The N-P type co-doping of Nb and Re atoms retained the continuous band characteristics of the original monolayer WS while also providing the high carrier mobility of graphene, yielding an excellent multipurpose material for manufacturing high-speed Schottky devices and efficient water-splitting H evolution catalysts.