HYDROGENATION OF AROMATIC-HYDROCARBONS OVER SUPPORTED PT CATALYSTS .2. TOLUENE HYDROGENATION

被引:167
作者
LIN, SD
VANNICE, MA
机构
[1] Department of Chemical Engineering, Pennsylvania State University, University Park
关键词
D O I
10.1006/jcat.1993.1298
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
Vapor-phase toluene hydrogenation was investigated over Pt supported on SiO2, η-Al2O3, SiO2 · Al2O3 and TiO2. As with benzene, activation energies and reaction orders had no dependence on the support. The EA values were 12 ± 2 kcal/mol and the partial pressure dependence on toluene was near zero, i.e. essentially the same as for benzene; however, the H2 pressure dependence increased from less than 0.7 at 333 K to over unity at 373 K. The turnover frequencies were four times higher with the most acidic support compared to the least acidic support, i.e., at 333 K under 50 Torr toluene and 685 Torr H2, the TOF on 0.24% Pt/SiO2 · Al2O3 was 0.112 s-1, whereas it was 0.027s-1 on 0.96% Pt/SiO2. This rate enhancement is attributed to an additional hydrogenation reaction occurring via hydrogen spilling over onto the support and reacting with aromatic molecules adsorbed on acid sites on the oxide. Deactivation was less of a problem with toluene compared to benzene. © 1993 Academic Press, Inc.
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页码:554 / 562
页数:9
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