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Surface-mediated reductive carbonylation of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) studied by IR spectroscopy
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
2001-11-20
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
关键词[WOS]FISCHER-TROPSCH SYNTHESIS ; ORGANOMETALLIC SYNTHESIS ; COBALT CARBONYLS ; METAL-CATALYSTS ; CO ADSORPTION ; HIGH-YIELD ; REACTIVITY ; CLUSTERS ; SILICA ; HYDROFORMYLATION
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.
语种英语
WOS记录号WOS:000171993200028
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文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/138955
专题中国科学院大连化学物理研究所
作者单位Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
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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.
APA Huang, L,&Xu, YD.(2001).Surface-mediated reductive carbonylation of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) studied by IR spectroscopy.JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL,176(1-2),267-280.
MLA Huang, L,et al."Surface-mediated reductive carbonylation of SiO2-supported RuCl3 and Ru(NO)(NO3)(3) studied by IR spectroscopy".JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL 176.1-2(2001):267-280.
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