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DC Field | Value | Language |
---|---|---|
dc.citation.endPage | 14338 | - |
dc.citation.number | 38 | - |
dc.citation.startPage | 14329 | - |
dc.citation.title | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | - |
dc.citation.volume | 135 | - |
dc.contributor.author | Li, Hongjiao | - |
dc.contributor.author | Calle-Vallejo, Federico | - |
dc.contributor.author | Kolb, Manuel J. | - |
dc.contributor.author | Kwon, Youngkook | - |
dc.contributor.author | Li, Yongdan | - |
dc.contributor.author | Koper, Marc T. M. | - |
dc.date.accessioned | 2023-12-22T03:37:24Z | - |
dc.date.available | 2023-12-22T03:37:24Z | - |
dc.date.created | 2019-04-17 | - |
dc.date.issued | 2013-09 | - |
dc.description.abstract | A surface structural preference for (1 0 0) terraces of fcc metals is displayed by many bond-breaking or bond-making reactions in electrocatalysis. Here, this phenomenon is explored in the electrochemical oxidation of dimethyl ether (DME) on platinum. The elementary C-O bond-breaking step is identified and clarified by combining information obtained from single-crystal experiments and density functional theory (DFT) calculations. Experiments on Pt(1 0 0), Pt(5 1 0), and Pt(10 1 0) surfaces show that the surface structure sensitivity is due to the bond-breaking step, which is unfavorable on step sites. DFT calculations suggest that the precursor for the bond-breaking step is a CHOC adsorbate that preferentially adsorbs on a square ensemble of four neighboring atoms on Pt(1 0 0) terraces, named as "the active site". Step sites fail to strongly adsorb CHOC and are, therefore, ineffective in breaking C-O bonds, resulting in a decrease in activity on surfaces with increasing step density. Our combined experimental and computational results allow the formulation of a new mechanism for the electro-oxidation of DME as well as a simple general formula for the activity of different surfaces toward electrocatalytic reactions that prefer (1 0 0) terrace active sites. | - |
dc.identifier.bibliographicCitation | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.135, no.38, pp.14329 - 14338 | - |
dc.identifier.doi | 10.1021/ja406655q | - |
dc.identifier.issn | 0002-7863 | - |
dc.identifier.scopusid | 2-s2.0-84884854858 | - |
dc.identifier.uri | https://scholarworks.unist.ac.kr/handle/201301/26538 | - |
dc.identifier.url | https://pubs.acs.org/doi/10.1021/ja406655q | - |
dc.identifier.wosid | 000330162900054 | - |
dc.language | 영어 | - |
dc.publisher | AMER CHEMICAL SOC | - |
dc.title | Why (100) Terraces Break and Make Bonds: Oxidation of Dimethyl Ether on Platinum Single-Crystal Electrodes | - |
dc.type | Article | - |
dc.description.isOpenAccess | FALSE | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Multidisciplinary | - |
dc.relation.journalResearchArea | Chemistry | - |
dc.type.docType | Article | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
dc.subject.keywordPlus | AUGMENTED-WAVE METHOD | - |
dc.subject.keywordPlus | ACID-SOLUTIONS | - |
dc.subject.keywordPlus | ETHANOL ELECTROOXIDATION | - |
dc.subject.keywordPlus | ALKALINE-SOLUTION | - |
dc.subject.keywordPlus | SURFACE-STRUCTURE | - |
dc.subject.keywordPlus | OXYGEN REDUCTION | - |
dc.subject.keywordPlus | FUEL-CELL | - |
dc.subject.keywordPlus | CO | - |
dc.subject.keywordPlus | ADSORPTION | - |
dc.subject.keywordPlus | PT(100) | - |
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