Transient Mechanistic Studies of Methane Steam Reforming over Ceria-Promoted Rh/Al2O3 Catalysts

被引:11
|
作者
Duarte, R. B. [1 ]
Olea, M. [2 ]
Iro, E.
Sasaki, T. [3 ]
Itako, K. [3 ]
van Bokhoven, J. A. [1 ,4 ]
机构
[1] Swiss Fed Inst Technol, Inst Chem & Bioengn, CH-8093 Zurich, Switzerland
[2] Univ Teesside, Sch Sci & Engn, Middlesbrough TS1 3BA, Cleveland, England
[3] Univ Tokyo, Grad Sch Frontier Sci, Dept Complex Sci & Engn, Chiba 2778561, Japan
[4] Paul Scherrer Inst, Lab Catalysis & Sustainable Chem, CH-5232 Villigen, Switzerland
关键词
carbon; cerium; hydrogen; kinetics; supported catalysts; GAS SHIFT REACTION; CARBON-MONOXIDE OXIDATION; HETEROGENEOUS CATALYSIS; RESPONSE METHOD; CHEMICAL CONVERSION; MANGANESE-DIOXIDE; NICKEL-CATALYSTS; NOBLE-METALS; HYDROGEN; RHODIUM;
D O I
10.1002/cctc.201402388
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
Transient-pulse experiments in temporal-analysis-of-product (TAP) and conventional mode were performed to determine elementary reaction steps involved in the methane steam reforming reaction over Rh/Al2O3 and Rh/12CeO(2)-Al2O3. TAP pulse experiments demonstrated that both catalysts dissociate methane at 773K leading to hydrogen, carbon, and CHx adspecies. Conventional transient pulse experiments with alternating methane/argon and water pulses with a delay between them of 86, 73, and 5s, respectively, showed that the reactivity of adspecies over the promoted and nonpromoted catalysts decrease with time. Ceria catalyzes the oxidation of carbon species by water.
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页码:2898 / 2903
页数:6
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