Adjacent diatomic Cu1N3/Mo1S2 entities decorated carbon nitride for markedly enhanced photocatalytic hydrogen generation

Abstract

The regulation of the electronic structure of graphitic carbon nitride (CN) has been considered as one of the most promising methods to improve its photocatalytic efficiency. However, how to adjust effectively the electronic structure remains a great challenge. Herein, we pioneered a microwave-assisted solvothermal sulphidation strategy for the preparation of Cu1N3-linked Mo1S2 adjacent diatomic entities decorated CN (Cu1N3/Mo1S2/CN) through the enabled sulphidation around single Cu atom by the super hot spots owing to the localized surface plasmon resonance effect. The electronic structure of CN is regulated by the synergistic effect of the adjacent diatomic metal Cu and Mo, which not only makes the conduction band of the catalyst closer to the Fermi level, but also improves the charge transfer of CN. As a result, Under visible light irradiation and atmosphere conditions, the H2 generation rate (HER) of the Cu1N3/Mo1S2/CN catalyst reaches as high as 6.14 mmol g-1h−1, which is 85 times higher than that onbulk CN. It was highlighted that the introduced Cu1N3-linked Mo1S2 adjacent diatomic entities act as modulator to efficiently tune the electronic structure of the CN semiconductor, rather than as active sites, and for all samples, the deposited Pt is requested to act as active sites for H2 production. This work not only provides enlightenment for the development of an outstanding non-precious metals modified CN-based photocatalyst for solar hydrogen production, but also provides a new avenue for the design of diverse adjacent diatomic catalysts towards various transformations.