Construction of dual defect mediated Z-scheme photocatalysts for enhanced photocatalytic hydrogen evolution

Abstract

The construction of Z-scheme system is a promising approach for photocatalytic hydrogen evolution (PHE). In this study, we fabricated a direct Z-scheme system consisting of defect-rich g-C3N4 nanosheets (DR-CNNS) crumpled nanosheets with defect-rich TiO2 (DR-TiO2) nanoparticles via a dual defective strategy. The optimized dual-defective rich TiO2/CNNS composite showed a superior PHE rate of ˜651.79 μmol/h with a turnover frequency of ˜419.3 h−1 as well as high stability and recyclability, which presented the highest value in single defective TiO2 or g-C3N4-based photocatalysts families reported previously. Furthermore, this protocol could also be extended to synthesize other dual defective g-C3N4/oxides (ZnO, SnO2, etc.) heterostructures. The improved photocatalytic performances could be ascribed to the following aspects: (1) rich dual defect, narrowing the band gap and providing more reactive sites for PHE; (2) intimate interface, facilitating interfacial migration and utilization of photogenerated charges; (3) Z-scheme structure, accelerating photogenerated electron-hole pair separation and thus leading to more efficient PHE. Our work highlights the critical role of defects in construction of Z-scheme system and provides the possibility of utilizing dual defective g-C3N4-based systems for other photocatalytic applications including CO2 reduction and water purification.