Photocatalytic co-production of hydrogen gas and N-benzylidenebenzylamine over high-quality 2D layered In4/3P2Se6 nanosheets

Abstract

The concurrent photocatalytic synthesis of hydrogen gas and high-valued chemicals over two-dimensional semiconductors is extremely attractive to alleviate global energy and environmental concerns through directly using sunlight. Herein, a novel layered In_4/3P₂Se₆ nanosheet is synthesized by a space confined chemical vapor conversion method, and it acts as a dual-functional photocatalyst to deliver the co-production of hydrogen gas and N-benzylidenebenzylamine from water reduction and selective benzylamine oxidation. The simultaneous yield of hydrogen gas and N-benzylidenebenzylamine is 895 μmol g⁻¹ and 681 μmol g⁻¹, respectively, within 16-hour continuous reaction involving a small amount of water in acetonitrile solvent. Moreover, 97.4% N-benzylidenebenzylamine selectivity from benzylamine oxidation can be achieved with continuous 10 hour-reaction only in acetonitrile solvent under ambient conditions. Further in situ electron paramagnetic resonance measurements and reaction optimization tests reveal that the reaction mechanism strongly relies on the conditions over the In_4/3P₂Se₆ nanosheet photocatalyst.