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题名: Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts
作者: Wang, Y;  Luo, HY;  Liang, DB;  Bao, XH
关键词: mechanism ;  acetaldehyde ;  ethanol ;  Rh-based catalysts ;  CO-TPD
刊名: JOURNAL OF CATALYSIS
发表日期: 2000-11-15
DOI: 10.1006/jcat.2000.3026
卷: 196, 期:1, 页:46-55
收录类别: SCI
文章类型: Article
部门归属: 5
项目归属: 502
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Engineering, Chemical
研究领域[WOS]: Chemistry ;  Engineering
英文摘要: Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts were investigated by the TPR (temperature programmed reaction) method, and the active sites were studied by CO-TPD, TPSR (temperature programmed surface reaction of preadsorbed CO by H-2) and XPS techniques. The TPR results indicated that ethanol and acetaldehyde might be formed through different intermediates, whereas ethanol and methanol might result from the same intermediate. Results of CO-TPD, TPSR, and XPS showed that on the Rh-based catalyst, the structure of the active sites for the formation of C-2-oxygenates is ((RhxRhy+)-Rh-0)-O-Mn+ (M=Mn or Zr, x>>y, 2 less than or equal ton less than or equal to4). The tilt-adsorbed CO species is the main precursor for CO dissociation and the precursor for the formation of ethanol and methanol. Most of the linear and geminal adsorbed CO species desorbed below 500 K. Based on the suggested model of the active sites, detailed mechanisms for the formation of acetaldehyde and ethanol are proposed. Ethanol is formed by direct hydrogenation of the tilt-adsorbed CO molecules, followed by CH2 insertion into the surface CH2-O species and the succeeding hydrogenation step. Acetaldehyde is formed through CO insertion into the surface CH3-Rh species followed by hydrogenation, and the role of the promoters was to stabilize the intermediate of the surface acetyl species. (C) 2000 Academic Press.
关键词[WOS]: CARBON-MONOXIDE HYDROGENATION ;  SUPPORTED RHODIUM CATALYSTS ;  SIO2-SUPPORTED RH ;  SPECTROSCOPIC EVIDENCE ;  RH/SIO2 CATALYSTS ;  SYNGAS CONVERSION ;  PROMOTED RHODIUM ;  CO+H-2 REACTION ;  PRESSURE ;  MNO
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000165598200005
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/91401
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:
Wang, Y,Luo, HY,Liang, DB,et al. Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts[J]. JOURNAL OF CATALYSIS,2000,196(1):46-55.
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