In-situ Construction of Sulfur-doped g-C3N4/defective g-C3N4 Iso-type Step-scheme Heterojunction for Boosting Photocatalytic H2 Evolution

The rational construction of a high-efficiency stepscheme heterojunctions is an effective strategy to accelerate the photocatalytic H-2. Unfortunately, the variant energy-level matching between two different semiconductor confers limited the photocatalytic performance. Herein, a newfangled graphitic-carbon nitride (g-C3N4) based isotype step-scheme heterojunction, which consists of sulfur-doped and defective active sites in one microstructural unit, is successfully developed by in-situ polymerizing N,N-dimethylformamide (DMF) and urea, accompanied by sulfur (S) powder. Therein, the polymerization between the amino groups of DMF and the amide group of urea endows the formation of rich defects. The propultion exhibits a significantly enlarged surface area, thus leading to the more exposed catalytically active sites. Most importantly, the simultaneous introduction of S-doping and defects in the units of g-C3N4 also results in a significant improvement in the separation, transfer and recombination efficiency of photo-excited electron-hole pairs. Therefore, the resulting isotype step-scheme heterojunction possesses a superior photocatalytic H-2 evolution activity in comparison with pristine g-C3N4. The newly afforded metal-free isotype step-scheme heterojunction in this work will supply a new insight into coupling strategies of heteroatoms doping and defect engineering for various photocatalytic systems.

Automated summary

A novel isotype step-scheme heterojunction with rich defects and catalytically active sites is successfully developed by polymerizing N,N-dimethylformamide (DMF) and urea with sulfur (S) powder. The simultaneous introduction of S-doping and defects greatly improves the separation, transfer, and recombination efficiency of photo-excited electron-hole pairs.