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Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts; Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts
Wang, Y; Luo, HY; Liang, DB; Bao, XH
关键词Mechanism Mechanism Acetaldehyde Acetaldehyde Ethanol Ethanol Rh-based Catalysts Rh-based Catalysts Co-tpd Co-tpd
刊名JOURNAL OF CATALYSIS ; JOURNAL OF CATALYSIS
2000-11-15 ; 2000-11-15
DOI10.1006/jcat.2000.3026 ; 10.1006/jcat.2000.3026
196期:1页:46-55
收录类别SCI ; SCI
文章类型Article ; Article
部门归属5 ; 5
项目归属502 ; 502
WOS标题词Science & Technology ; Science & Technology ; Physical Sciences ; Physical Sciences ; Technology ; Technology
类目[WOS]Chemistry, Physical ; Chemistry, Physical ; Engineering, Chemical ; Engineering, Chemical
研究领域[WOS]Chemistry ; Chemistry ; Engineering ; Engineering
关键词[WOS]CARBON-MONOXIDE HYDROGENATION ; CARBON-MONOXIDE HYDROGENATION ; SUPPORTED RHODIUM CATALYSTS ; SUPPORTED RHODIUM CATALYSTS ; SIO2-SUPPORTED RH ; SIO2-SUPPORTED RH ; SPECTROSCOPIC EVIDENCE ; SPECTROSCOPIC EVIDENCE ; RH/SIO2 CATALYSTS ; RH/SIO2 CATALYSTS ; SYNGAS CONVERSION ; SYNGAS CONVERSION ; PROMOTED RHODIUM ; PROMOTED RHODIUM ; CO+H-2 REACTION ; CO+H-2 REACTION ; PRESSURE ; PRESSURE ; MNO ; MNO
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.; 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.
语种英语 ; 英语
原文出处查看原文 ; 查看原文
WOS记录号WOS:000165598200005 ; WOS:000165598200005
引用统计
被引频次:50[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/91401
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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GB/T 7714
Wang, Y,Luo, HY,Liang, DB,et al. Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts, Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts[J]. JOURNAL OF CATALYSIS, JOURNAL OF CATALYSIS,2000, 2000,196, 196(1):46-55, 46-55.
APA Wang, Y,Luo, HY,Liang, DB,&Bao, XH.(2000).Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts.JOURNAL OF CATALYSIS,196(1),46-55.
MLA Wang, Y,et al."Different mechanisms for the formation of acetaldehyde and ethanol on the Rh-based catalysts".JOURNAL OF CATALYSIS 196.1(2000):46-55.
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