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 $${{\mbox{g}}}_{{\mbox{cat}}}^{-1}$$ 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. The design of multifunction reactive sites is pivotal for cascade reaction. Here, the authors prepared a high-entropy photocatalyst that enables direct C–N coupling of alcohols with NH3 to form imines, achieving high benzyl alcohol-to-imine yield.