Evaluation of the role of the metal-support interfacial centers in the dry reforming of methane on alumina-supported rhodium catalysts

Evaluation of the role of the metal-support interfacial centers in the dry reforming of methane on alumina-supported rhodium catalysts
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DOI:
10.1006/jcat.1999.2752
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发表时间:
2000-03-10
影响因子:
7.3
通讯作者:
Rodríguez-Ramos, I
Rodríguez-Ramos, I
中科院分区:
化学1区
文献类型:
--
作者:
Ferreira-Aparicio, P;Fernandez-Garcia, M;Rodríguez-Ramos, I

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研究了一系列Al(2)O(3)负载Rh-Cu催化剂上CH(4)与CO(2)的干重整反应。已发现该反应通过双功能机制在这些系统上进行,其中甲烷上的活化发生在铑相上,而二氧化碳通过甲酸酯中间体在载体表面上活化。添加金属,如铜,对甲烷活化无活性,使我们能够评估界面Rh-Al(2)O(3)位点在反应中的作用。铜的存在降低了催化剂的稳定性,尽管它对每个表面暴露位点的初始活性没有任何影响。这表明甲烷干重整反应不是一个结构敏感的反应,催化活性,在很大程度上受氧化铝载体,是依赖于表面暴露的铑中心的数量。(C)北京大学出版社.
The reforming of CH(4) with CO(2) (dry reforming) has been studied on a series of Al(2)O(3)-supported Rh-Cu catalysts. The reaction has been found to proceed on these systems through a bifunctional mechanism, in which the activation on methane takes place on the rhodium phase while carbon dioxide is activated on the support surface via formate intermediates. The addition of a metal, such as copper, inactive for methane activation, has allowed us to evaluate the role of the interfacial Rh-Al(2)O(3) sites in the reaction. The presence of copper reduces the stability of the catalysts, though it does not have any effect on the initial activity per surface exposed site. It indicates that the dry reforming of methane is not a structure-sensitive reaction and that catalytic activity, largely affected by the alumina support, is dependent on the number of surface exposed rhodium centers. (C) 2000 Academic Press.