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Incorporating metal nanodots (NDs) into heterostructures for high charge separation and transfer capacities is one of the most effective strategies for improving their photocatalytic activities. However, controlling the space distribution of metal NDs for optimizing charge transport pathways remains a significant challenge, particularly in two-dimensional (2D) face-to-face heterostructures. Herein, we develop a simple targeted self-reduction strategy for selectively loading Ru NDs onto the Ti3−xC2Ty (TC) surface of 2D TC/g-C3N4 (CN) heterojunction based on the reductive Ti vacancy defects creatively increased during the preparation of TC/CN by reducing calcination. Notably, the optimized Ru/TC/CN photocatalyst exhibits an outstanding H2 evolution rate of 3.21 mmol·g−1h−1 and a high apparent quantum efficiency of 30.9% at 380 nm, which is contributed by the unidirectional transfer of the photogenerated electrons from CN to Ru active sites (CN → TC → Ru) and the suppressed backflow of electrons from Ru sites to CN, as revealed by comprehensive characterizations and density functional theory (DFT) calculations. This work provides a novel strategy for synthesizing the highly efficient photocatalysts with a controllable charge transfer paths, which will boost the development of photocatalysis. [ABSTRACT FROM AUTHOR]

[Display omitted] • Integration of S-scheme/Schottky junctions and oxygen vacancies on SrTiO 3 is constructed. • Formed junctions enable the transfer of charges with direction. • Designed hybrid dramatically improves photocatalytic H 2 evolution activity. • Large-scale photocatalytic device (20 cm × 20 cm) is successfully demonstrated. The interfacial design and defect engineering are of huge interest for achieving efficient photocatalytic H 2 evolution using solar energy. In this work, we successfully integrated the Schottky junction and S-scheme heterojunction with oxygen vacancies to achieve the defective Ru/SrTiO 3 /TiO 2 hybrid photocatalyst. As verified by experimental studies, these junctions with defects fully exploit the benefits of interfacial charge separation and transport. It is demonstrated that the designed hybrid exhibits dramatically enhanced photocatalytic H 2 evolution rate with respect to pristine SrTiO 3 , high apparent quantum efficiency at 365 nm irradiation as well as excellent stability. Furthermore, the Ru/SrTiO 3 /TiO 2 based device photocatalyst also displays the excellent H 2 evolution activity with easy recycle nature. This finding provides a newfangled thought for developing highly efficient hybrid materials for photocatalytic H 2 evolution. [ABSTRACT FROM AUTHOR]

Integrating 2D layered bimetallic cobalt molybdenum sulfide (CMS) with 3D TiO 2 hollow shells (THS) dramatically boosts the photocatalytic H 2 evolution rate. • A special 2D-3D Co 1.62 Mo 6 S 8 -TiO 2 film-shell photocatalyst is constructed. • This hybrid nanostructure endows improved light harvesting capacity. • The introduction of 2D film boosts the charge separation efficiency. • A H 2 evolution rate as high as 44.43 mmol h−1 g−1 is achieved. Integrating two-dimensional (2D) transition metal sulfide (TMS) nanostructures with the semiconductor materials is one strategy to improve their photocatalytic performance. Herein, for the first time, supporting noble-metal-free Co 1.62 Mo 6 S 8 (CMS) with a 2D structure on three-dimensional (3D) TiO 2 hollow shells (THS) is developed to construct the special CMS/THS 2D-3D film-shell photocatalyst. Based on a range of spectroscopic and electrochemical techniques, such structure can accelerate charge separation and transfer, provide abundant active sites for water reduction, and enhance light harvesting capacity through light scattering and slow photon effects. As expected, the optimized CMS/THS photocatalyst exhibits excellent photocatalytic H 2 evolution activity and good stability under simulated solar light irradiation, whose rate is 39 times higher than that of THS and even much better than those of CoS 2 /THS and MoS 2 /THS. This strategy may be applicable to construct other various 2D-3D integrated nanostructures for excellent performance. [ABSTRACT FROM AUTHOR]