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Quantification of Interfacial pH Variation at Molecular Length Scales Using a Concurrent Non-Faradaic Reaction
DC Field | Value | Language |
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dc.contributor.author | Ryu, Jaeyune | - |
dc.contributor.author | Wuttig, Anna | - |
dc.contributor.author | Surendranath, Yogesh | - |
dc.date.accessioned | 2023-05-03T05:45:55Z | - |
dc.date.available | 2023-05-03T05:45:55Z | - |
dc.date.created | 2023-05-01 | - |
dc.date.created | 2023-05-01 | - |
dc.date.created | 2023-05-01 | - |
dc.date.issued | 2018-07 | - |
dc.identifier.citation | Angewandte Chemie International Edition, Vol.57 No.30, pp.9300-9304 | - |
dc.identifier.issn | 1433-7851 | - |
dc.identifier.uri | https://hdl.handle.net/10371/191797 | - |
dc.description.abstract | We quantified changes in interfacial pH local to the electrochemical double layer during electrocatalysis by using a concurrent non-faradaic probe reaction. In the absence of electrocatalysis, nanostructured Pt/C surfaces mediate the reaction of H-2 with cis-2-butene-1,4-diol to form a mixture of 1,4-butanediol and n-butanol with selectivity that is linearly dependent on the bulk solution pHvalue. We show that kinetic branching occurs from a common surface-bound intermediate, ensuring that this probe reaction is uniquely sensitive to the interfacial pHvalue within molecular length scales of the surface. We used the pH-dependent selectivity of this reaction to track changes in interfacial pH during concurrent hydrogen oxidation electrocatalysis and found that the local pHvalue can vary dramatically (>3units) relative to the bulk value even at modest current densities in well-buffered electrolytes. This study highlights the key role of interfacial pH variation in modulating inner-sphere electrocatalysis. | - |
dc.language | 영어 | - |
dc.publisher | John Wiley & Sons Ltd. | - |
dc.title | Quantification of Interfacial pH Variation at Molecular Length Scales Using a Concurrent Non-Faradaic Reaction | - |
dc.type | Article | - |
dc.identifier.doi | 10.1002/anie.201802756 | - |
dc.citation.journaltitle | Angewandte Chemie International Edition | - |
dc.identifier.wosid | 000438712600011 | - |
dc.identifier.scopusid | 2-s2.0-85050031503 | - |
dc.citation.endpage | 9304 | - |
dc.citation.number | 30 | - |
dc.citation.startpage | 9300 | - |
dc.citation.volume | 57 | - |
dc.description.isOpenAccess | Y | - |
dc.contributor.affiliatedAuthor | Ryu, Jaeyune | - |
dc.type.docType | Article | - |
dc.description.journalClass | 1 | - |
dc.subject.keywordPlus | COUPLED ELECTRON-TRANSFER | - |
dc.subject.keywordPlus | ELECTROCHEMICAL REDUCTION | - |
dc.subject.keywordPlus | CARBON-DIOXIDE | - |
dc.subject.keywordPlus | CO2 REDUCTION | - |
dc.subject.keywordPlus | SELECTIVITY | - |
dc.subject.keywordPlus | SURFACES | - |
dc.subject.keywordAuthor | electrocatalysis | - |
dc.subject.keywordAuthor | electrochemical double layers | - |
dc.subject.keywordAuthor | hydrogenation | - |
dc.subject.keywordAuthor | interfacial pH | - |
dc.subject.keywordAuthor | proton-coupled electron transfer | - |
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