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Gold nanofilm redox catalysis for oxygen reduction at soft interfaces

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dc.contributor.author Smirnov, Evgeny
dc.contributor.author Peljo, Pekka
dc.contributor.author Scanlon, Micheál D.
dc.contributor.author Peljo, Pekka
dc.contributor.author Girault, Hubert H.
dc.date.accessioned 2020-01-14T14:40:01Z
dc.date.available 2020-01-14T14:40:01Z
dc.date.issued 2016
dc.identifier.citation Smirnov, Evgeny; Peljo, Pekka; Scanlon, Micheál D. and Girault, Hubert H. (2016) 'Gold nanofilm redox catalysis for oxygen reduction at soft interfaces'. Electrochimica Acta, 197 :362-373. en_US
dc.identifier.uri http://hdl.handle.net/10344/8371
dc.description peer-reviewed en_US
dc.description.abstract .Functionalization of a soft or liquid-liquid interface by a one gold nanoparticle thick “nanofilm” provides a conductive pathway to facilitate interfacial electron transfer from a lipophilic electron donor to a hydrophilic electron acceptor in a process known as interfacial redox catalysis. The gold nanoparticles in the nanofilm are charged by Fermi level equilibration with the lipophilic electron donor and act as an interfacial reservoir of electrons. Additional thermodynamic driving force can be provided by electrochemically polarising the interface. Using these principles, the biphasic reduction of oxygen by a lipophilic electron donor, decamethylferrocene, dissolved in α,α,α-trifluorotoluene was catalysed at a gold nanoparticle nanofilm modified water-oil interface. A recently developed microinjection technique was utilised to modify the interface reproducibly with the mirror-like gold nanoparticle nanofilm, while the oxidised electron donor species and the reduction product, hydrogen peroxide, were detected by ion transfer voltammetry and UV/vis spectroscopy, respectively. Metallization of the soft interface allowed the biphasic oxygen reduction reaction to proceed via an alternative mechanism with enhanced kinetics and at a significantly lower overpotential in comparison to a bare soft interface. Weaker lipophilic reductants, such as ferrocene, were capable of charging the interfacial gold nanoparticle nanofilm but did not have sufficient thermodynamic driving force to significantly elicit biphasic oxygen reduction en_US
dc.language.iso eng en_US
dc.publisher Elsevier en_US
dc.relation 13SIRG2137 en_US
dc.relation.ispartofseries Electrochimica Acta;197 pp. 362-373
dc.relation.uri http://www.sciencedirect.com/science/article/pii/S001346861530685X doi=10.1016/j.electacta.2015.10.104
dc.relation.uri http://dx.doi.org/10.1016/j.electacta.2015.10.104
dc.rights This is the author’s version of a work that was accepted for publication in Electrochimica Acta. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Electrochimica Acta, 197, pp.362-373,http://dx.doi.org/10.1016/j.electacta.2015.10.104 en_US
dc.subject gold nanoparticles en_US
dc.subject soft interfaces en_US
dc.subject electron transfer en_US
dc.subject electrocatalysis en_US
dc.subject oxygen reduction reaction en_US
dc.title Gold nanofilm redox catalysis for oxygen reduction at soft interfaces en_US
dc.type info:eu-repo/semantics/article en_US
dc.type.supercollection all_ul_research en_US
dc.type.supercollection ul_published_reviewed en_US
dc.date.updated 2020-01-10T16:16:33Z
dc.description.version ACCEPTED
dc.identifier.doi 10.1016/j.electacta.2015.10.104
dc.contributor.sponsor Swiss National Science Foundation en_US
dc.relation.projectid 2000-20-152-557/1 en_US
dc.relation.projectid 13/SIRG/2137 en_US
dc.rights.accessrights info:eu-repo/semantics/openAccess en_US
dc.internal.rssid 2697080
dc.internal.copyrightchecked Yes
dc.identifier.journaltitle Electrochimica Acta
dc.description.status peer-reviewed


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