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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
KeywordMethanol Oxidation Bulk Gold O-2 Activation Hydroperoxyl Water Density Functional Theory
Source PublicationACS CATALYSIS
2013-08-01
DOI10.1021/cs400344r
Volume3Issue:8Pages:1693-1699
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordCHEMICAL-VAPOR-DEPOSITION ; TRANSITION-METAL SURFACES ; DENSITY-FUNCTIONAL THEORY ; LOW-TEMPERATURE OXIDATION ; SELECTIVE OXIDATION ; AEROBIC OXIDATION ; CO OXIDATION ; O-2 DISSOCIATION ; PHASE OXIDATION ; SUPPORTED GOLD
AbstractTo 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.
Language英语
WOS IDWOS:000322852900002
Citation statistics
Cited Times:59[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/137735
Collection中国科学院大连化学物理研究所
Affiliation1.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
GB/T 7714
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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