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题名: IR studies on the preservation of RhCo3 clusters on the surface of SiO2
作者: Huang, L
关键词: SiO2-physisorbed RhCo3(CO)(12) ;  stabilization of RhCo3 ;  regeneration and dissociation of RhCo3(CO)(12)
刊名: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
发表日期: 1996-10-10
卷: 112, 期:1, 页:69-83
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: The adsorption of RhCo3(CO)(12) on the SiO2 surface, and the interactions of SiO2-suppoaed RhCo3(CO)(12) and SiO2-supported RhCo3(CO)(12)-derived catalyst with CO have been studied at room temperature by IR spectroscopy. A strong physisorption of RhCo3(CO)(12) on partially dehydroxylated SiO2 occurs spontaneously, which results in a dramatic change of carbonyl spectral pattern and downward shifts of both linear and bridged carbonyl bands. The SiO2-grafted RhCo3(CO)(12) is characterized by two carbonyl bands at 2028 and 1830 cm(-1). These observations may be interpreted in terms of a nucleophilic attack of surface oxygen containing groups on the cobalt atoms of the bimetallic cluster. Following decarbonylation of RhCo3(CO)(12)/SiO2 under H-2 at 623 K, the resulting catalyst surface can be recarbonylated by to regenerate the starting bimetallic carbonyl cluster which is then gradually disintegrated to Rh-6(CO)(16) and Co-2(CO)(8) under CO. In parallel, the precursor RhCo3(CO)(12)/SiO2 itself readily reacts with CO to dissociate to Rh-6(CO)(16) and Co-4(CO)(12). The reaction mixture is not only identified on the surface during exposure to CO but also extracted from the surface into the organic solvent. The results suggest that the RhCo, cluster framework is preserved on SiO, despite that the precursor has undergone the severe thermal decarbonylation treatment, and that RhCo3(CO)(12) is regenerated by CO adsorption. A tight SiO, surface-bound RhCo3 cluster is proposed for the supported bimetallic catalyst in terms of cluster-support interaction. In addition, the discrepancy between the regenerated supported RhCo3(CO)(12) and the precursor during the dissociation processes is discussed.
关键词[WOS]: PARTIALLY-HYDROXYLATED MAGNESIA ;  BIMETALLIC CARBONYL CLUSTERS ;  TEMPERATURE-PROGRAMMED REDUCTION ;  ORGANOMETALLIC CHEMISTRY ;  OXIDE SUPPORTS ;  HYDRATED SILICA ;  CATALYSTS ;  COBALT ;  REACTIVITY ;  DECOMPOSITION
语种: 英语
WOS记录号: WOS:A1996VM67500009
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/142782
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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Recommended Citation:
Huang, L. IR studies on the preservation of RhCo3 clusters on the surface of SiO2[J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL,1996,112(1):69-83.
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