High-entropy photocatalyst enabling collaborative cascade C-N coupling for converting benzyl alcohol to imine

The selective conversion of biomass-derived alcohols to nitrogen-containing organic chemicals, such as the highly valuable imine, is a significant challenge due to the complex tandem process of C-N coupling and multiple reaction pathways. The photocatalytic coupling of biomass-derived alcohols with NH₃ using renewable energy offers a sustainable way to produce imines, but requires the development of suitable photocatalysts. In this work, we present a promising high-entropy sulfide photocatalyst (NiSnCaZnInS) with integrated multifunctional sites. Using benzyl alcohol (BA) as an example, we achieved an imine yield of 1240 μmol ${\text{g}}_{\text{cat}}^{-1}$ for 5 hours, with a selectivity of 91.7%. The photocatalytic performance can be attributed to the special configuration of the high-entropy surface, which provides ideal catalytic sites for the cascade coupling reaction. This work highlights the great potential of high-entropy materials in photocatalytic reactions, providing a sustainable and effective approach to the photocatalytic conversion of biomass derivatives into valuable chemicals.