Construction of an all-organic S-scheme heterostructure based on PEDOT immobilized g-C3N4 nanosheets by electrostatic self-assembly with enhanced visible-light photocatalytic hydrogen production

Inspired by photosynthesis in nature, exploring all-organic S-scheme heterojunction photocatalysts for efficient H2 production is of great significance in addressing energy shortage issues. In this paper, poly(3,4-ethylenedioxythiophene) (PEDOT) immobilized g-C3N4(CN) nanosheets were constructed by an electrostatic self-assembly strategy to obtain an all-organic S-scheme heterojunction, significantly enhancing the visible-light photocatalytic H2 production performance of g-C3N4. The optimized 5PEDOT/CN exhibits the highest H2 production rate of 3.15 mmol g−1h−1, a 31.5-fold enhancement over pristine CN. According to the staggered energy band positions of two components and the results of electron spin resonance tests, the S-scheme heterojunction electron-transfer mechanism is confirmed, which greatly facilitates the spatial charge separation and retains the strong reducing ability of high-energy potential electrons for efficient photocatalytic H2 production. Based on the results of FT-IR spectra, XPS spectra, fluorescence spectra, hydroxyl radical tests and time-resolved photoluminescence spectra, it is confirmed that the significantly improved photocatalytic activity is mainly attributed to the enhanced charge separation by the S-scheme heterojunction and the tightly contacted interface dependent on N···S interactions in PEDOT immobilized CN nanosheet heterojunctions, along with the enhanced visible-light absorption ability. This work presents a novel approach to the design and fabrication of all-organic S-scheme heterojunction photocatalysts for solar-light-driven energy production.