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题名: Surface-mediated reductive carbonylation of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) studied by IR spectroscopy
作者: Huang, L;  Xu, YD
关键词: SiO2 ;  RuCl3 ;  Ru(NO)(NO3)(3) ;  N2O ;  reductive carbonylation ;  reduction of NO
刊名: JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
发表日期: 2001-11-20
卷: 176, 期:1-2, 页:267-280
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 surface-mediated reductive carbonylation Of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) has been studied by IR spectroscopy. Hydrated RuCl3/SiO2 reacts readily with CO (100-700 Torr) to form a mixture of Ru(CO)Cl-2(HOSi)(3) and Ru(CO)(2)Cl-2(HOSi)(2) at 25 degreesC, and a mixture of Ru(CO)Cl-2(HOSi)(3), Ru(CO)(2)Cl-2(HOSi)(2), Ru(CO)(3)Cl-2(HOSi) (major product) and [Ru(CO)(3)Cl-2](2) at 100 degreesC. Hydrated Ru(NO)(NO3)(3)/SiO2 reacts readily with CO to give a mixture of Ru(CO)(2)(OSi)(2) and Ru(CO)(3)(OSi)(2) at 25 degreesC. At 100 degreesC, hydrated Ru(NO)(NO3)(3)/SiO2 is converted to a mixture of Ru(CO)(2)(OSi)(2) and Ru(CO)(3)(OSi)(2) under 100 Torr of CO, and a mixture of Ru-3(CO)(12) (good yield) and RU(CO)(3)(OSi)(2) under 700 Torr of CO. All these results are demonstrated by surface IR spectra and extraction experiments with organic solvents. While the carbonylation of hydrated RU(NO)(NO3)(3)/SiO2 proceeds, the stoichiometric reductions of NO3- and NO: 2NO(3)(-) + 3CO + 2HOSi --> 2NO + 3CO(2) + H2O + 2OSi(-) and 2NO + CO --> N2O + CO2 are suggested to occur on the surface, according to gaseous IR observation. The proportion of ruthenium(II) tricarbonyl species is found to increase with the increases of carbonylation temperature and CO pressure. In addition, the detrimental effect of calcination of RuCl3/SiO2 and Ru(NO)(NO3)(3)/SiO2 at 400 degreesC on the reductive carbonylation is discussed. (C) 2001 Elsevier Science B.V. All rights reserved.
关键词[WOS]: FISCHER-TROPSCH SYNTHESIS ;  ORGANOMETALLIC SYNTHESIS ;  COBALT CARBONYLS ;  METAL-CATALYSTS ;  CO ADSORPTION ;  HIGH-YIELD ;  REACTIVITY ;  CLUSTERS ;  SILICA ;  HYDROFORMYLATION
语种: 英语
WOS记录号: WOS:000171993200028
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/138955
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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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Huang, L,Xu, YD. Surface-mediated reductive carbonylation of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) studied by IR spectroscopy[J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL,2001,176(1-2):267-280.
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