Palladium-bismuth intermetallic and surface-poisoned catalysts for the semi-hydrogenation of 2-methyl-3-butyn-2-ol

被引:52
作者
Cherkasov, Nikolay [1 ]
Ibhadon, Alex . [1 ]
McCue, Alan J. [2 ]
Anderson, James A. [2 ]
Johnston, Shaun K. [1 ]
机构
[1] Univ Hull, Catalysis & Reactor Engn Res Grp, Dept Chem & Sch Biol Biomed & Environm Sci, Kingston Upon Hull HU6 7RX, N Humberside, England
[2] Univ Aberdeen, Dept Chem, Surface Chem & Catalysis Grp, Old Aberdeen AB24 3UE, Scotland
关键词
Heterogeneous catalysis; Alkynol; 2-Methyl-3-butyn-2-ol; Hydrogenation; Semi-hydrogenation; Palladium; Bismuth; LIQUID-PHASE HYDROGENATION; SELECTIVE HYDROGENATION; MONTE-CARLO; BI; ACETYLENE; CARBON; SIZE; HYDRODECHLORINATION; TOXICITY; KINETICS;
D O I
10.1016/j.apcata.2015.02.038
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 effects of poisoning of Pd catalysts with Bland annealing in a polyol (ethylene glycol) were studied on the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). An increase in the Pd:Bi ratio from 7 to 1 in the Bi-poisoned catalysts decreased the hydrogenation activity due to blocking of active sites, but increased maximum alkene yield from 91.5% for the Pd catalyst to 94-96% for all Bi-poisoned Pd catalysts, by decreasing the adsorption energy of alkene molecules and suppressing the formation of beta-hydride phase. Annealing of the catalysts induced the formation of intermetallic phases and decreased its activity due to sintering of the catalytic particles and low activity of intermetallic compounds. Lang-muir-Hinshelwood kinetic modelling of the experimental data showed that poisoning of Pd with Bi changed the relative adsorption constants of organic species suggesting ligand effects at high Bi content. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:22 / 30
页数:9
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