Hydrogenolysis of alkanes: reactions of n-butane on Ru/zeolite catalysts

被引:5
|
作者
Bond, Geoffrey C. [1 ]
Garcia, Juan J. [1 ]
机构
[1] Brunel Univ, Dept Chem, Uxbridge UB8 3PH, Middx, England
关键词
TREATED RU/TIO2 CATALYSTS; RU/AL2O3; CATALYSTS; METAL-CATALYSTS; RUTHENIUM; KINETICS;
D O I
10.1039/c7cy00677b
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
Ru/13X zeolite catalysts containing 0.6, 2 and 5.7% Ru prepared by reduction or decomposition of the hexammine complex are active and stable for n-butane hydrogenolysis between 400 and 460 K, and show similar activation energies (150-160 kJ mol(-1)) and orders of reaction(-1.5 to -2 in H-2; 0.5-0.65 in n-butane); product selectivities show weak dependence on temperature and H-2 pressure, with preference for terminal bond scission. Oxidising either the decomposed or the reduced catalysts gave a marked increase in activity, a lower activation energy (120-130 kJ mol-1), higher orders of reaction in H-2 (similar to-0.9), lower orders in n-butane (similar to 0.2) and product selectivities that showed greater change with temperature and H-2 pressure; terminal bond scission was >90%. The change in character with oxidation was attributed to weaker H-2 chemisorption and a higher concentration of partially dehydrogenated C-4 species; the active phase may consist of very small particles of RuO2 confined within the supercages of the zeolite.
引用
收藏
页码:5294 / 5300
页数:7
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