LAUSR

Abstract Simultaneously exploration control of energy band, layer structure and vacancy defect of semiconductor photocatalysts for hydrogen (H2) evolution is highly desirable. For this purpose, the ultrathin graphitic carbon nitride (ug-C3N4) are prepared by intercalated hydrogen bond effect of NO3− for the first time reported. More importantly, the thickness, band gap energy, specific surface area and nitrogen vacancy intensity of ug-C3N4 nanosheets can be controlled by the concentration of NO3− in the inserted layer. The method not only endow ug-C3N4 nanosheets with super large specific surface area and nitrogen vacancy-rich that provide more active sites and speed up the photogenerated charge transfer, but also possess suitable conduction band position and thus more conducive to H2 production. The photocatalytic performance of ug-C3N4 for H2 evolution (836.3 µmol h−1 g−1) and 2-Mercaptobenzothiazole (MBT) decomposition (84%) is significantly enhanced by energy band, layer structure and vacancy defect optimization, which is over 4.0 and 1.75 times higher than the bulk g-C3N4 powder. We firmly believe that the work emblems a significant step toward control engineering for energy conversion and environmental pollution.