Cocatalyst-modified In 2 S 3 photocatalysts for C–N coupling of amines integrated with H 2 evolution

Abstract

The dual function of visible-light-driven cooperative production of imine and H 2 is realized on oxidative cocatalyst PdS-modified In 2 S 3 nanospheres, which fully utilizes the synergistic potential of the photoredox system. Photocatalytic hydrogen (H 2 ) production coupled with selective oxidation of organic compounds into high-value-added organic intermediates has expansive prospects in the utilization and transformation of solar energy, which meets the development requirements of green chemistry. In this work, high-efficiency hole cocatalyst PdS-decorated In 2 S 3 flower-like microspheres are fabricated for the effective visible-light-driven C–N coupling of amines to imines coupled with H 2 evolution. Owing to the establishment of the internal electric field, which further boosts the transfer of photoexcited holes to PdS, PdS–In 2 S 3 exhibits distinctly enhanced photocatalytic redox performance, which is 39.8 times higher for H 2 and 14.3 times higher for N -benzylidenebenzylamine than that of the blank In 2 S 3 , along with high selectivity and stability. Furthermore, the practicability of dehydrogenation coupling of various aromatic amines to the corresponding C–N coupling products on PdS–In 2 S 3 has been demonstrated and a plausible reaction mechanism has been proposed. This work is anticipated to stimulate further interest in establishing an innovative photoredox platform for selective organic synthesis coupled with H 2 evolution in a green and sustainable way.