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

被引:6
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
相关论文
共 12 条
[1]  
Bond G.C., 2005, Metal-catalysed reactions of hydrocarbons: metals and alloys
[2]  
Bond G. C., 2005, METAL CATALYSED REAC
[3]   Compensation phenomena in heterogeneous catalysis: General principles and a possible explanation [J].
Bond, GC ;
Keane, MA ;
Kral, H ;
Lercher, JA .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2000, 42 (03) :323-383
[4]   Kinetics of alkane reactions on metal catalysts: activation energies and the compensation effect [J].
Bond, GC .
CATALYSIS TODAY, 1999, 49 (1-3) :41-48
[5]  
Bond GC, 1996, J CHEM TECHNOL BIOT, V65, P15
[6]   STUDIES ON RUTHENIUM CATALYSTS .2. OXIDES OF THE 1ST ROW TRANSITION-ELEMENTS AS MODIFIERS OF A RU/SIO2 CATALYST [J].
BOND, GC ;
YAHYA, R .
JOURNAL OF MOLECULAR CATALYSIS, 1991, 69 (01) :75-93
[7]   HYDROGENOLYSIS OF ALKANES .2. HYDROGENOLYSIS OF N-BUTANE OVER VARIOUSLY TREATED RU/TIO2 CATALYSTS [J].
BOND, GC ;
XU, Y .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1984, 80 :3103-3118
[8]   CATALYTIC AND STRUCTURAL-PROPERTIES OF RUTHENIUM BIMETALLIC CATALYSTS - KINETICS OF HYDROGENOLYSIS OF LOWER ALKANES ON VARIOUSLY PRETREATED RU/AL2O3 CATALYSTS [J].
BOND, GC ;
SLAA, JC .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1995, 98 (02) :81-99
[9]  
BOND GC, 2005, METAL CATALYSED REAC, pCH5
[10]   HYDROGENOLYSIS OF ALKANES .3. HYDROGENOLYSIS OF NORMAL-HEXANE AND METHYLCYCLOPENTANE OVER VARIOUSLY TREATED RU/TIO2 CATALYSTS [J].
BURCH, R ;
BOND, GC ;
RAJARAM, RR .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1986, 82 :1985-1998