Detailed kinetic study of fischer-tropsch synthesis on co/zro2/sio2 catalyst i. analysis of reaction pathways
文献类型:期刊论文
作者 | Chang, J; Teng, BT; Bai, L; Zhang, RL; Chen, JG; Xu, YY; Xiang, HW; Li, YW; Sun, YH |
刊名 | Chinese journal of catalysis
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出版日期 | 2005-07-01 |
卷号 | 26期号:7页码:614-620 |
关键词 | Cobalt-based catalyst Fischer-tropsch synthesis Reaction kinetics Reaction pathway Energetic analysis Unsteady state experiment |
ISSN号 | 0253-9837 |
通讯作者 | Chang, j() |
英文摘要 | Mechanistic analysis for the fischer-tropsch (f-t) synthesis has been conducted to resolve the tedious task in assembling a mass of model equations in its kinetic studies. using the unity bond index-quadratic exponential potential (ubi-qep) method, it is found that on the model cobalt-based catalyst co(0001) surface, the surface carbide mechanism via ch2,s insertion into the oxygen-free intermediates is energetically favorable. the dissociation of co and the first hydrogenation of surface carbon have higher active barriers than the other elementary steps. the unsteady state experiments show that the formation of h2o is the most important way to remove the surface oxygen at the f-t synthesis temperature on co/zro2/sio2. the formation and consequent hydrogenation of c, is the rate- determining step in the reaction pathway, while the c-c coupling is a relatively faster elementary reaction. there are more carbon pools for the methane formation, and the deviation of the methane product from the classical anderson- schulz-flory product distribution might be due to the multiform carbon pools. combining the results of theoretical and experimental analysis, a framework of f-t synthesis mechanistic models is obtained. this framework is similar to the surface carbide mechanism, in which the co, dissociation or the surface carbon hydrogenation is the rate- determining step, and the ch2,s insertion produces the final hydrocarbons. but the detail forms of the oxygen-free intermediates (alkyl or alkylidene) in the carbon chain propagation cannot be discriminated. this will be resolved by the kinetic analysis in the next part of this series work. |
WOS关键词 | CO HYDROGENATION ; HYDROCARBON SYNTHESIS ; SUPPORTED COBALT ; SPECTROSCOPY ; ADSORPTION ; MECHANISM |
WOS研究方向 | Chemistry ; Engineering |
WOS类目 | Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical |
语种 | 英语 |
WOS记录号 | WOS:000230982300019 |
出版者 | SCIENCE PRESS |
URI标识 | http://www.irgrid.ac.cn/handle/1471x/2377765 |
专题 | 中国科学院大学 |
通讯作者 | Chang, J |
作者单位 | 1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100039, Peoples R China |
推荐引用方式 GB/T 7714 | Chang, J,Teng, BT,Bai, L,et al. Detailed kinetic study of fischer-tropsch synthesis on co/zro2/sio2 catalyst i. analysis of reaction pathways[J]. Chinese journal of catalysis,2005,26(7):614-620. |
APA | Chang, J.,Teng, BT.,Bai, L.,Zhang, RL.,Chen, JG.,...&Sun, YH.(2005).Detailed kinetic study of fischer-tropsch synthesis on co/zro2/sio2 catalyst i. analysis of reaction pathways.Chinese journal of catalysis,26(7),614-620. |
MLA | Chang, J,et al."Detailed kinetic study of fischer-tropsch synthesis on co/zro2/sio2 catalyst i. analysis of reaction pathways".Chinese journal of catalysis 26.7(2005):614-620. |
入库方式: iSwitch采集
来源:中国科学院大学
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