Physically and chemically mixed TiO2-supported Pd and Au catalysts: unexpected synergistic effects on selective hydrogenation of citral in supercritical CO2

被引:65
作者
Liu, Ruixia [1 ]
Yu, Yancun [1 ]
Yoshida, Kazuki [2 ]
Li, Guiming [3 ]
Jiang, Haoxi [3 ]
Zhang, Minhua [3 ]
Zhao, Fengyu [1 ]
Fujita, Shin-ichiro [2 ]
Arai, Masahiko [2 ]
机构
[1] Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Peoples R China
[2] Hokkaido Univ, Div Chem Proc Engn, Grad Sch Engn, Sapporo, Hokkaido 0608628, Japan
[3] Tianjin Univ, Key Lab Green Chem Technol, Minist Educ Res & Dev, Ctr Petrochem Technol, Tianjin 300072, Peoples R China
关键词
Bimetallic catalysts; Palladium; Gold; Synergistic effects; Hydrogen spillover; Hydrogenation; Citral; Supercritical CO2; CARBON-DIOXIDE; GOLD CATALYSTS; DICHLORODIFLUOROMETHANE CFC-12; ACETYLENE HYDROGENATION; AROMATICS HYDROGENATION; MOLECULAR-INTERACTIONS; PHASE HYDROGENATION; SUPPORTED CATALYSTS; NANOPARTICLES; OXIDATION;
D O I
10.1016/j.jcat.2009.11.007
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The selective hydrogenation of citral was studied with various TiO2-supported monometallic and bimetallic Pd and Au catalysts and their physical mixtures in supercritical CO2 (scCO(2)). Significant synergistic effects appeared when active Pd species was chemically or physically mixed with less active Au species. The total rate of conversion was greatly enhanced and the selectivity to citronellal (CAL) was improved. The physical properties of those catalysts were characterized by TEM, HRTEM-EDS, XPS, and UV/Vis and their features of H-2 desorption were examined by TPD. The physical and chemical characterization results were used to discuss the reasons for the unexpected synergistic effects observed. The same selective hydrogenation was also conducted in a conventional non-polar organic solvent of n-hexane to examine the roles of scCO(2). The use of scCO(2) was effective for accelerating the hydrogenation of citral and improving the selectivity to CAL (c) 2009 Elsevier Inc. All rights reserved.
引用
收藏
页码:191 / 200
页数:10
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