LDH表面微结构调控Ru单原子光催化剂加氢选择性的研究

选择性催化加氢是极为重要的工业基本单元反应，世界上大约有25%的化工过程的其中一步需要用到加氢工艺。在加氢体系中存在多个可加氢的官能团时，在传统催化剂上往往发生低选择性加氢或过度加氢的现象，高选择性地获得目标产物仍存在巨大挑战。基于申请人最新的研究结果，为解决催化加氢的选择性问题，本项目提出基于LDH负载Ru单原子催化剂在可见光下实现选择性加氢的新思路：1）利用LDH表面的缺陷及官能团等微结构，调控负载的Ru单原子电子结构实现靶向官能团的优先吸附形成表面化合物，进而吸光发生电子跃迁实现活化；2）通过在LDH表面构筑协同反应位，辅助实现吸附、活化及脱附过程。本项目的实施将对进一步设计高效、高选择性的金属加氢催化剂及理解加氢反应机理提供实验及理论依据。

Selective catalytic hydrogenation is an extremely important industrial basic unit reaction, and about 25% of the chemical industrial processes in the world requires hydrogenation step. When there are multiple reducible functional groups co-exist in the reaction system, the phenomenon of low-selective hydrogenation or over hydrogenation is often occurred on traditional catalysts. The synthesis of target product in a highly selective manner is still a great challenge. Based on our latest study, we proposes a new idea for the realization of selective hydrogenation under visible light on Ru/LDH single atomic catalyst: 1) The electronic structure of Ru single-atom catalyst is adjusted by utilizing the microstructures such as defects and surface groups of LDH surface to achieve the priority adsorption of the targeting group, which then forms a Ru-surface complex compound and realize activation under light irradiation. 2) The adsorption, activation and desorption processes are assisted by constructing a synergistic reaction site on the surface of LDH. The implementation of this project will provide experimental and theoretical basis for the further design of highly efficient and highly selective metal hydrogenation catalysts and profound understanding of hydrogenation reaction mechanism.