Defect engineering and Ni promoter synergistically accelerating electron transfer to Ru^(0) sites in UiO-66(Ce) for dicyclopentadiene hydrogenation under mild condition  

作　　者：Rushuo Li Tao Ban Danfeng Zhao Jing Lin Zhiyuan Liu Linmeng Wang Xiubing Huang Zhiping Tao Ge Wang 

机构地区：[1]Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory of Function Materials for Molecule and Structure Construction, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China [2]Sinopec Research Institute of Petroleum Processing Co., Ltd., Beijing, 100083, China

出　　处：《Nano Research》2024年第11期9550-9563,共14页纳米研究（英文版）

基　　金：supported by the National Key Research and Development Program of China(No.2021YFB3500700);the National Natural Science Foundation of China(No.51972024);the Natural Science Foundation of Guangdong Province(No.2022A1515010185).

摘　　要：Olefin hydrogenation under mild condition is crucial and challenging for industrial applications. Herein, defective UiO-66(Ce) was constructed by using cyanuric acid as the molecular etching “scissors” and further to synthesize heterogeneous catalyst with highly dispersed RuNi nanoparticles (Ru1Ni1.5@UiO-66(Ce)-12 h). The construction of Ce-O-Ru/Ni heterogeneous interfaces and Ni–Ru bonds provide electron transfer channels from Ce-oxo clusters and Ni species to Ru species. Furthermore, the microenvironment and electronic structure of Ru0 active sites were synergistically regulated by adjusting the content of metal-organic frameworks (MOFs) defects and Ni promoter, thereby enhancing the adsorption and activation ability of H–H and C=C bonds. Therefore, Ru1Ni1.5@UiO-66(Ce)-12 h achieved dicyclopentadiene saturated hydrogenation (100% conversion) to tetrahydrodicyclopentadiene (∼ 100% selectivity) under mild condition (35℃, 1 MPa) with only 25 min. Meanwhile, the sample exhibited excellent structural stability after 6 cycles test. This study provides a promising strategy for the rational design of remarkable noble metal-based catalysts for practical applications.

关 键 词：metal-organic frameworks defect engineering Ni promoter electron-rich Ru^(0)active sites dicyclopentadiene hydrogenation 

分 类 号：O64[理学—物理化学]