DICP OpenIR
First-Principles Study on the Origin of the Different Selectivities for Methanol Steam Reforming on Cu(111) and Pd(111)
Gu, Xiang-Kui; Li, Wei-Xue1
刊名JOURNAL OF PHYSICAL CHEMISTRY C
2010-12-16
DOI10.1021/jp107678d
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
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
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.
语种英语
WOS记录号WOS:000284990800089
引用统计
被引频次:95[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/321008/141989
专题中国科学院大连化学物理研究所
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
推荐引用方式
GB/T 7714
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.
APA Gu, Xiang-Kui,&Li, Wei-Xue.(2010).First-Principles Study on the Origin of the Different Selectivities for Methanol Steam Reforming on Cu(111) and Pd(111).JOURNAL OF PHYSICAL CHEMISTRY C,114(49),21539-21547.
MLA Gu, Xiang-Kui,et al."First-Principles Study on the Origin of the Different Selectivities for Methanol Steam Reforming on Cu(111) and Pd(111)".JOURNAL OF PHYSICAL CHEMISTRY C 114.49(2010):21539-21547.
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Gu, Xiang-Kui]的文章
[Li, Wei-Xue]的文章
百度学术
百度学术中相似的文章
[Gu, Xiang-Kui]的文章
[Li, Wei-Xue]的文章
必应学术
必应学术中相似的文章
[Gu, Xiang-Kui]的文章
[Li, Wei-Xue]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。