Dong Yuan, Zhao Haoming, Liu Zhenjie, Yang Ming, Zhang Zhenlin, Zhu Ting, Cheng Hansong
Sustainable Energy Laboratory, Faculty of Materials Science and Chemistry, China University of Geosciences Wuhan 430074 P. R. China
Zhejiang Institute, China University of Geosciences Hangzhou 311305 P. R. China.
RSC Adv. 2020 Mar 17;10(19):11039-11045. doi: 10.1039/d0ra01277g. eCollection 2020 Mar 16.
The competitive adsorption of 8-methylquinoline (8-MQL) and partially hydrogenated product, 4H-8-MQL, was studied by performing a combination of experiments and first-principles calculations over a selected Ru catalyst. A series of hydrogenation reactions were conducted with 8-MQL and 4H-8-MQL as initial reactants, respectively. 8-MQL exhibits stronger adsorption on catalyst surface active sites compared with 4H-8-MQL and the massive adsorption of 8-MQL hampers the further adsorption of 4H-8-MQL. The effects of temperature, pressure and solvent on the selectivity in 8-MQL hydrogenation were investigated as well. Full hydrogenation of 8-MQL to 10H-8-MQL was achieved within 120 min when the catalyst dosage increased from 5 wt% to 7 wt% under 160 °C and a hydrogen pressure of 7 MPa. The electronic charge of the N-heteroatom in 8-MQL and 4H-8-MQL was analyzed and the adsorption geometries of 8-MQL and 4H-8-MQL on the Ru(001) surface were optimized by DFT calculations to explain the competitive adsorption behaviors of 8-MQL and 4H-8-MQL.
