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题名: Rh-Decorated Cu Alloy Catalyst for Improved C-2 Oxygenate Formation from Syngas
作者: Zhao, Yong-Hui1;  Yang, Ming-Mei1;  Sun, Dapeng1;  Su, Hai-Yan1;  Sun, Keju1;  Ma, Xiufang1;  Bao, Xinhe1;  Li, Wei-Xue1
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2011-09-22
DOI: 10.1021/jp204961g
卷: 115, 期:37, 页:18247-18256
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: C-2 oxygenate (acetaldehyde, ethanol, etc.) formation from syngas (CO (+) H-2) is an important industrial process for the production of clean liquid energy fuels and valuable chemical feedstocks that are catalyzed industrially by Rh modified with Mn and Fe, etc. In an effort to identify catalysts based on less expensive metals and higher C-2 oxygenate selectivity, density functional theory (DFT) calculations were performed to tune the relative activity of the selectivity-determining steps, i.e., CO insertion in CHx, (x = 1, 2, 3) versus CHx, hydrogenation by changing composition and structure of material. We find that the Rh-decorated Cu alloy catalyst has significantly lower CO insertion barriers compared to pristine Rh(111) and vicinal Rh(553) surfaces, whereas the variation of CHx, hydrogenation barriers on the three surfaces is modest. A semiquantitative kinetic analysis based on DFT calculations shows that the C-2 oxygenate selectivity on RhCu(111) is substantially improved, with the production rate of C-2 oxygenates slightly higher than CH4, under experimental conditions, compared with Rh(111) and Rh(553) that are highly selective to CH4,. Our calculations suggest that the improved C-2 oxygenate selectivity on the RhCu alloy is primarily due to the fact that CO insertion is rather sensitive, whereas hydrogenation is insensitive to the ensemble effect. Furthermore, the Rh-decorated Cu alloy has stronger resistance toward coking and lower constituent cost compared to pure Rh catalysts and is thus a promising candidate for an improved C-2 oxygenate synthesis catalyst.
关键词[WOS]: DENSITY-FUNCTIONAL THEORY ;  CARBON-MONOXIDE HYDROGENATION ;  PROMOTED RH/SIO2 CATALYSTS ;  AUGMENTED-WAVE METHOD ;  MINIMUM ENERGY PATHS ;  ELASTIC BAND METHOD ;  METAL-SURFACES ;  CO HYDROGENATION ;  SUPPORTED RHODIUM ;  ALKALI PROMOTION
语种: 英语
WOS记录号: WOS:000294875200028
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/142678
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:
Zhao, Yong-Hui,Yang, Ming-Mei,Sun, Dapeng,et al. Rh-Decorated Cu Alloy Catalyst for Improved C-2 Oxygenate Formation from Syngas[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2011,115(37):18247-18256.
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