Electrogenerated chemiluminescence at droplet-modified electrodes: towards biphasic pK(a) measurement via proton-coupled electron transfer at liquid vertical bar liquid interfaces

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dc.contributor.authorLledo-Fernandez, Carlos
dc.contributor.authorHatay, Imren
dc.contributor.authorBall, Michael J.
dc.contributor.authorGreenway, Gillian M.
dc.contributor.authorWadhawan, Jay
dc.date.accessioned2020-03-26T17:38:32Z
dc.date.available2020-03-26T17:38:32Z
dc.date.issued2009
dc.departmentSelçuk Üniversitesien_US
dc.description.abstractThis preliminary work reports, for the first time, electrogenerated chemiluminescence (ECL) at droplet-modified electrodes. The system involves oxidation of aqueous tris(2,2'-bipyridyl) ruthenium(II) ions at a glassy carbon electrode on which a random array of microdroplets of a highly hydrophobic tertiary amine (trioctylamine) are immobilised. Luminescence, produced via electron transfer over the cupola surface of the droplets from the oil to aqueous tris(2,2'-bipyridyl) ruthenium(III) ions synthesised via intra muros electrochemical oxidation at the uncovered parts of the electrode surface, is demonstrated. The extent of ECL production is shown to be dependent on the degree of interfacial protonation, with a proton-coupled biphasic electron transfer reaction occurring when the liquid vertical bar liquid interface is fully protonated, changing to a biphasic outer-sphere electron transfer mechanism when the interface is fully deprotonated. The competition and gradual dominance of one of these extreme mechanisms under intermediate interfacial protonation conditions thence enables the sensitive, kinetic estimation of the biphasic pK(a).en_US
dc.description.sponsorshipHull University; Selcuk University of KonyaSelcuk University; The Nuffield Foundationen_US
dc.description.sponsorshipC.L.-F. and G. M. G. express gratitude to Hull University for funding via the Graduate Teaching Assistance Scheme. IH thanks Selcuk University of Konya for funding her work at Hull University via the ERASMUS European Exchange programme. M. J. B. gratefully thanks The Nuffield Foundation for financing his summer studentship via their Undergraduate Research Bursary scheme (GR/N URB/33192). J. W. is indebted to Hull University for financial support via a start- up grant, and thanks Evangelia Christoforou for undertaking some experiments.en_US
dc.identifier.doi10.1039/b810844gen_US
dc.identifier.endpage759en_US
dc.identifier.issn1144-0546en_US
dc.identifier.issn1369-9261en_US
dc.identifier.issue4en_US
dc.identifier.scopusqualityQ2en_US
dc.identifier.startpage749en_US
dc.identifier.urihttps://dx.doi.org/10.1039/b810844g
dc.identifier.urihttps://hdl.handle.net/20.500.12395/23507
dc.identifier.volume33en_US
dc.identifier.wosWOS:000264978900010en_US
dc.identifier.wosqualityQ1en_US
dc.indekslendigikaynakWeb of Scienceen_US
dc.indekslendigikaynakScopusen_US
dc.language.isoenen_US
dc.publisherROYAL SOC CHEMISTRYen_US
dc.relation.ispartofNEW JOURNAL OF CHEMISTRYen_US
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanıen_US
dc.rightsinfo:eu-repo/semantics/closedAccessen_US
dc.selcuk20240510_oaigen_US
dc.titleElectrogenerated chemiluminescence at droplet-modified electrodes: towards biphasic pK(a) measurement via proton-coupled electron transfer at liquid vertical bar liquid interfacesen_US
dc.typeArticleen_US

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