The liquid-phase hydrogenation of 1-heptyne over Pd-Au/TiO2 catalysts prepared by the combination of incipient wetness impregnation and deposition-precipitation

被引:37
作者
Kittisakmontree, Prathan [1 ]
Pongthawornsakun, Boontida [1 ]
Yoshida, Hiroshi [2 ]
Fujita, Shin-ichiro [2 ]
Arai, Masahiko [2 ]
Panpranot, Joongjai [1 ]
机构
[1] Chulalongkorn Univ, Dept Chem Engn, Ctr Excellence Catalysis & Catalyt React Engn, Fac Engn, Bangkok 10330, Thailand
[2] Hokkaido Univ, Fac Engn, Div Chem Proc Engn, Sapporo, Hokkaido 0608628, Japan
基金
日本学术振兴会;
关键词
1-Heptyne; Selective hydrogenation; Liquid-phase hydrogenation; Pd-Au bimetallic catalysts; FLAME SPRAY-PYROLYSIS; AU-PD NANOPARTICLES; SELECTIVE HYDROGENATION; PD/SIO2; CATALYSTS; HEAT-TREATMENT; GOLD; PALLADIUM; ACETYLENE; CO; TEMPERATURE;
D O I
10.1016/j.jcat.2012.10.007
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
TiO2-supported Pd-Au catalysts were prepared with Pd (0.5 wt%) by impregnation and then Au (1.0 wt%) by deposition-precipitation (Au/Pd/TiO2) and vice versa (Pd/Au/TiO2). For the former sample, the state of dispersion of Pd on TiO2 changed during the loading of Au, resulting in the formation of small Au-Pd alloy particles and thus changing the electronic properties of Pd species. The alloy formation was not clearly detected on the Pd/Au/TiO2, and the electronic properties of Pd were not so different from those of monometallic Pd/TiO2. All the catalysts were selective to 1-heptene (> 95%) until close to the complete conversion of 1-heptyne. However, the selectivity of 1-heptene drastically decreased to 0% (which was further hydrogenated to heptane) in 120 min for the Au/Pd/TiO2 while it still remained > 60% for the Pd/Au/TiO2 similar to the monometallic Pd/TiO2 catalyst. The rate of 1-heptene hydrogenation (in the second step) did not depend on the Pd dispersion but was found to be greatly enhanced as the Pd species became electron-rich in the Au-Pd alloy particles. The modification of Pd species by Au was less significant for the first step of hydrogenation of 1-heptyne to 1-heptene. (c) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:155 / 164
页数:10
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