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题名: A Water-Promoted Mechanism of Alcohol Oxidation on a Au(111) Surface: Understanding the Catalytic Behavior of Bulk Gold
作者: 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
发表日期: 2013-08-01
DOI: 10.1021/cs400344r
卷: 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
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.
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
语种: 英语
WOS记录号: WOS:000322852900002
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/137735
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.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

Recommended Citation:
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.
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