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题名: Promotion effect of support calcination on ethanol production from CO hydrogenation over Rh/Fe/Al2O3 catalysts
作者: Chen, Weimiao1;  Ding, Yunjie1, 2;  Song, Xiangeng1, 3;  Wang, Tao1;  Luo, Hongyuan1
关键词: Rhodium ;  Alumina ;  Iron ;  Carbon monoxide hydrogenation ;  Calcination temperature ;  Ethanol
刊名: APPLIED CATALYSIS A-GENERAL
发表日期: 2011-11-04
DOI: 10.1016/j.apcata.2011.08.044
卷: 407, 期:1-2, 页:231-237
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Life Sciences & Biomedicine
类目[WOS]: Chemistry, Physical ;  Environmental Sciences
研究领域[WOS]: Chemistry ;  Environmental Sciences & Ecology
英文摘要: A series of Rh/Fe/Al2O3 catalysts, in which the Al2O3 supports were calcined at different temperatures, were prepared by a sequential impregnation method. The catalysts were tested by CO hydrogenation and characterized by N-2 adsorption-desorption, X-ray diffraction (XRD), CO pulse chemisorption, temperature programmed surface reaction (TPSR) and temperature programmed reduction (TPR) techniques. The activity of ethanol formation was the highest when the catalyst support was calcined at 800 degrees C, while that of methanol formation increased continuously with the calcination temperature of the support. According to the commonly accepted mechanism of C-2-oxygenates formation, CO conversion followed three separate pathways after CO dissociation, and our results suggested that the activity towards CO insertion and dissociation increased gradually with the calcination temperature, but began to decrease at 900 degrees C. On the other hand, direct hydrogenation of CO to methanol was still increasing at 900 degrees C. These observations were in agreement with TPSR results. Dispersion of the Rh or Fe species was not impaired, and even improved, with the declining of the surface area of the support due to high temperature calcination. TPR results revealed that Rh-Fe interaction was strengthened after calcination, due to a lowering in surface hydroxyl reactivity of the support and an increase of the Rh-Fe interface area. As a result, the amount of Rh-Fe-O sites for CO dissociation and insertion increased with the calcination temperature, giving rise to the increase in ethanol formation activity. However, an over-strong Rh-Fe interaction would be resulted when the catalyst support was calcined at 900 degrees C, and this would cause more Fe species to be reduced, which would then cover the Rh sites. Consequently. CO uptake as well as dissociation and insertion of CO would decrease, leading to more CO molecules being hydrogenated directly to methanol, thus causing a decrease in the selectivity of ethanol formation. (C) 2011 Elsevier B.V. All rights reserved.
关键词[WOS]: RHODIUM CATALYSTS ;  FISCHER-TROPSCH ;  CARBON-MONOXIDE ;  RH CATALYSTS ;  C-2-OXYGENATES SYNTHESIS ;  SYNGAS CONVERSION ;  SYNTHESIS GAS ;  H-2/CO RATIO ;  OXIDE ;  IRON
语种: 英语
WOS记录号: WOS:000297234400028
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/142508
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, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Chinese Acad Sci, Grad Sch, Beijing 100039, Peoples R China

Recommended Citation:
Chen, Weimiao,Ding, Yunjie,Song, Xiangeng,et al. Promotion effect of support calcination on ethanol production from CO hydrogenation over Rh/Fe/Al2O3 catalysts[J]. APPLIED CATALYSIS A-GENERAL,2011,407(1-2):231-237.
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