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题名: First-Principles Study on the Origin of the Different Selectivities for Methanol Steam Reforming on Cu(111) and Pd(111)
作者: Gu, Xiang-Kui;  Li, Wei-Xue1
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2010-12-16
DOI: 10.1021/jp107678d
卷: 114, 期:49, 页:21539-21547
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: Methanol steam reforming (MSR) is an important industrial process for hydrogen production, and fundamental understanding of the reaction mechanism is crucial to improve the catalytic activity and selectivity. In the present work, we present a comparative mechanistic study of the MSR reaction on two key model systems, Cu(111) and Pd(111), with distinct selectivity using density functional theory calculations. We find that, on Cu(111), methanol dehydrogenation to formaldehyde is favorable first through the O-H bond scission, and the final products are dominated by carbon dioxide and hydrogen. On Pd(111), formaldehyde is also found to be an important intermediate; however, it comes through the C-H bond breaking first, and the final products are mainly CO and hydrogen. We find that the distinct selectivity on the Cu( Ill) and Pd(Ill) surfaces originates from the different reactivities of HCHO on the two surfaces. On Cu(111), HCHO tends to react with the hydroxyl to form hydroxymethoxy followed by its decomposition to CO2. In contrast, direct dehydrogenation of HCHO to CO is favorable on Pd(111). Finally, we find that there is a good linear correlation between the transition-state energies and the final-state energies for the elementary reactions involved in the MSR reaction, which may be useful for computational design and optimization of the catalysts.
关键词[WOS]: GAS SHIFT REACTION ;  DENSITY-FUNCTIONAL THEORY ;  TOTAL-ENERGY CALCULATIONS ;  COPPER-BASED CATALYSTS ;  ZINC-OXIDE CATALYSTS ;  ELASTIC BAND METHOD ;  WAVE BASIS-SET ;  LOW-TEMPERATURE ;  FUEL-CELLS ;  CU/ZNO/AL2O3 CATALYSTS
语种: 英语
WOS记录号: WOS:000284990800089
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141989
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
2.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret & Computat Chem, Dalian 116023, Peoples R China

Recommended Citation:
Gu, Xiang-Kui,Li, Wei-Xue. First-Principles Study on the Origin of the Different Selectivities for Methanol Steam Reforming on Cu(111) and Pd(111)[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2010,114(49):21539-21547.
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