Abstract
The development of new photoactive materials is of great practical significance for the construction of high-performance photoanodes to achieve highly efficient photoelectrochemical (PEC) water decomposition. Herein, we develop a facile ethanol-assisted hydrothermal method for in-situ growth of chalcogen vacancy-rich (VX, X: S/Se/Te)ReX2on carbon cloth to construct novel self-supporting ReX2-nphotoanodes. PEC tests coupled with ultrafast transient absorption spectroscopy investigated the mechanism by which VXregulates the charge decay dynamics of ReX2-nphotoanode and revealed the effective trapping behavior of VXon the microsecond scale after being excited by light. ReS2-n, ReSe2-n and ReTe2-n photoanodes achieve high photocurrent densities and the optimization effect of VX engineering on carrier transport has been validated by both DFT calculations and experimental results, with the introduced trap states addressing the ultrafast relaxation of photogenerated carriers caused by the narrow band gap. The research provides a novel strategy for the design and synthesis of ReX2 nanomaterials, decodes the carrier dynamics behind the enhancement of PEC activity of photoanodes modified by vacancy engineering, and provides valuable guidance for realizing high-efficiency PEC water oxidation, and which will greatly enrich the application of ReX2 in nanoelectronics, optoelectronics, and energy environmental devices.
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