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A Water-Promoted Mechanism of Alcohol Oxidation on a Au(111) Surface: Understanding the Catalytic Behavior of Bulk Gold
Chang, Chun-Ran1,2; Yang, Xiao-Feng1,2,3; Long, Bo1,2; Li, Jun1,2
关键词Methanol Oxidation Bulk Gold O-2 Activation Hydroperoxyl Water Density Functional Theory
刊名ACS CATALYSIS
2013-08-01
DOI10.1021/cs400344r
3期:8页:1693-1699
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Chemistry, Physical
研究领域[WOS]Chemistry
关键词[WOS]CHEMICAL-VAPOR-DEPOSITION ; TRANSITION-METAL SURFACES ; DENSITY-FUNCTIONAL THEORY ; LOW-TEMPERATURE OXIDATION ; SELECTIVE OXIDATION ; AEROBIC OXIDATION ; CO OXIDATION ; O-2 DISSOCIATION ; PHASE OXIDATION ; SUPPORTED GOLD
英文摘要To understand the catalytic mechanism of alcohol oxidation with molecular oxygen on bulk metallic gold catalysts, we have systematically studied the oxidative dehydrogenation of methanol on Au(111) using density functional theory. It is found that molecular oxygen can be activated via a hydroperoxyl (OOH) intermediate produced by abstracting a hydrogen atom from co-adsorbed methanol or water. Interestingly, extra water molecules significantly promote the hydrogen-transfer reactions between CH3OH center dot center dot center dot O-2 and H2O center dot center dot center dot O-2 co-adsorbates, lowering the activation barrier of OOH formation from similar to 0.90 to similar to 0.45 eV. The formed OOH intermediate either directly reacts with methanol to produce formaldehyde or dissociates into adsorbed atomic oxygen and hydroxyl. Further calculations demonstrate that the oxidative dehydrogenation of methanol by OOH, atomic oxygen, and hydroxyl is extremely facile with low barriers between 0.06 and 0.30 eV. These results provide an explanation for the activation mechanism of molecular oxygen on bulk gold and reveal a possible pathway for alcohol oxidation with dioxygen.
语种英语
WOS记录号WOS:000322852900002
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被引频次:54[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/321008/137735
专题中国科学院大连化学物理研究所
作者单位1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
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Chang, Chun-Ran,Yang, Xiao-Feng,Long, Bo,et al. A Water-Promoted Mechanism of Alcohol Oxidation on a Au(111) Surface: Understanding the Catalytic Behavior of Bulk Gold[J]. ACS CATALYSIS,2013,3(8):1693-1699.
APA Chang, Chun-Ran,Yang, Xiao-Feng,Long, Bo,&Li, Jun.(2013).A Water-Promoted Mechanism of Alcohol Oxidation on a Au(111) Surface: Understanding the Catalytic Behavior of Bulk Gold.ACS CATALYSIS,3(8),1693-1699.
MLA Chang, Chun-Ran,et al."A Water-Promoted Mechanism of Alcohol Oxidation on a Au(111) Surface: Understanding the Catalytic Behavior of Bulk Gold".ACS CATALYSIS 3.8(2013):1693-1699.
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