Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol‐Amine Coupling

Authors: Huimin Yi, Chenyi Wang, Baoxin Ge, Fangjie Xu, Pengyang Jiang, Min Zhou, Fangshu Xing, Caijin Huang

Published: 2025-03-23

DOI: 10.1002/smll.202500253

Source: Full article


Abstract

AbstractAchieving a precise understanding and accurate design of heterogeneous catalysts based on bioinspired principles is challenging yet crucial to digging out optimal materials for artificial catalysis. Here, an ADH‐mimicking dual‐site photocatalyst (YCuCdS) is developed, and demonstrates the powerful effects of atomic site configuration and proton transfer environments on alcohol‐amine coupling. Mechanism studies reveal that the alcohol substrate is effectively dehydrogenated at the Y sites, forming the carbonyl intermediates that rapidly experience condensation with the amine. Meanwhile, the released hydrogen species (Hads) migrate from adjacent Cu sites to active S atoms, promoting H2 production and hindering the over‐hydrogenation of imine. As a result, a high imine yield of 92% is achieved, along with an H2 production rate of 7400 µmol g−1 h−1. This work showcases an effective strategy for the design of heterogeneous catalysts with bioinspiration.