催化作用
化学
化学选择性
电子效应
氢
选择性
纳米颗粒
金属
铂金
密度泛函理论
多相催化
光化学
组合化学
有机化学
作者
Sai Zhang,Zhaoming Xia,Ting Ni,Zhiyun Zhang,Yuanyuan Ma,Yongquan Qu
标识
DOI:10.1016/j.jcat.2018.01.004
摘要
Abstract Selectively catalytic hydrogenation of various quinolines in the presence of other reducible groups into the 1,2,3,4-tetrahydroquinoline compounds under mild conditions is a particular challenge for the heterogeneous catalysts due to the natural chemical stability of quinolines and poor chemoselectivity. Pt-based catalysts generally deliver good catalytic activity and selectivity for hydrogenation of quinolines with other reducible groups. However, the over-hydrogenated by-products are also often observed. Herein, Pt nanoparticles supported on CeO2 nanorods (Pt/NR-CeO2) realized highly efficient and chemoselective hydrogenation of various functionalized quinolines at room temperature. The unusual catalytic performance can be attributed to the strong electronic metal-support interactions (EMSI) between Pt and NR-CeO2 with the abundant surface oxygen vacancy, resulting in the enhanced electronic density of Pt nanoparticles. Subsequently, the modulated electronic structure of Pt enables the efficient hydrogen activation at room temperature, leading to a TOF of 546 h−1 of Pt/NR-CeO2 for the selective hydrogenation of 6-chloroquinolines. Density functional theory calculations also reveal that the high electron density of Pt benefits the desorption of the hydrogenated products and thus avoids the over-hydrogenation effectively.
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