Methanol–steam reforming on Cu/ZnO/Al2O3 catalysts. Part 2. A comprehensive kinetic model

蒸汽重整 水煤气变换反应 甲醇 催化作用 一氧化碳 水煤气 格式化 化学工程 无机化学 吸附 脱氢 反应速率 反应机理 化学 甲醇重整装置 制氢 合成气 物理化学 有机化学 工程类
作者
Brant A. Peppley,J. C. Amphlett,Lyn M. Kearns,R. F. Mann
出处
期刊:Applied Catalysis A-general [Elsevier]
卷期号:179 (1-2): 31-49 被引量:513
标识
DOI:10.1016/s0926-860x(98)00299-3
摘要

Surface mechanisms for methanol–steam reforming on Cu/ZnO/Al2O3 catalysts are developed which account for all three of the possible overall reactions: methanol and steam reacting directly to form H2 and CO2, methanol decomposition to H2 and CO and the water-gas shift reaction. The elementary surface reactions used in developing the mechanisms were chosen based on a review of the extensive literature concerning methanol synthesis on Cu/ZnO/Al2O3 catalysts and the more limited literature specifically dealing with methanol–steam reforming. The key features of the mechanism are: (i) that hydrogen adsorption does not compete for the active sites which the oxygen-containing species adsorb on, (ii) there are separate active sites for the decomposition reaction distinct from the active sites for the methanol–steam reaction and the water-gas shift reaction, (iii) the rate-determining step (RDS) for both the methanol–steam reaction and the methanol decomposition reaction is the dehydrogenation of adsorbed methoxy groups and (iv) the RDS for the water-gas shift reaction is the formation of an intermediate formate species. A kinetic model was developed based on an analysis of the surface mechanism. Rate data were collected for a large range of conditions using a fixed-bed differential reactor. Parameter estimates for the kinetic model were obtained using multi-response least squares non-linear regression. The resultant model was able to accurately predict both the rates of production of hydrogen, carbon dioxide and of carbon monoxide for a wide range of operating conditions including pressures as high as 33 bar.
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