Charge separation, transmission, and light absorption properties are critical to determining the performance of photoelectrochemical (PEC) devices. An important strategy to control such properties is based on using heterostructured materials. Herein, a tunable zero-dimensional (0D)/two-dimensional (2D) heterostructure is designed based on quantum dots (QDs) and 2D nanosheets (NSs). Specifically, eco-friendly Zn-doped CuInS2 QDs prepared by hot injection were anchored on hierarchical (2D/2D) MoS2/rGO (MG) NSs through a facile sonication-assisted method to develop a 0D/2D/2D heterojunction-based photoelectrode for solar hydrogen production. The interfacial structure and band alignment between the proposed 0D QDs and 2D/2D MG NSs were engineered by modulating the Zn molar ratio during the QD synthesis. As proof of concept, the optimized 0D/2D/2D photoanode exhibits almost five times higher PEC activity than MG/CuInS2 and MoS2/Zn-CuInS2 NSs due to the enhanced light absorption, efficient charge separation, and transmission. Zn doping and the presence of graphene are essential in enhancing performance in the proposed heterostructure, reducing recombination of charge carriers, and improving sunlight absorption. This work shows how optimal band alignment control and carbon addition can facilitate charge transfer, enabling the development of highly efficient PEC devices based on 0D/2D/2D heterostructure nanocomposites.
Keywords: 0D/2D/2D heterostructures; charge transfer; doping; photoelectrochemical devices; quantum dots.