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Boosting water oxidation layer-by-layer

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dc.contributor.author Hidalgo-Acosta, Jonnathan C.
dc.contributor.author Scanlon, Micheál D.
dc.contributor.author Méndez, Manuel A.
dc.contributor.author Amstutz, Véronique
dc.contributor.author Vrubel, Heron
dc.contributor.author Opallo, Marcin
dc.contributor.author Girault, Hubert H.
dc.date.accessioned 2020-01-11T15:23:30Z
dc.date.available 2020-01-11T15:23:30Z
dc.date.issued 2016
dc.identifier.uri http://hdl.handle.net/10344/8370
dc.description peer-reviewed en_US
dc.description.abstract Electrocatalysis of water oxidation was achieved using fluorinated tin oxide (FTO) electrodes modified with layer-by-layer deposited films consisting of bilayers of negatively charged citrate-stabilized IrO2 NPs and positively charged poly(diallyldimethylammonium chloride) (PDDA) polymer. The IrO2 NP surface coverage can be fine-tuned by controlling the number of bilayers. The IrO2 NP films were amorphous, with the NPs therein being well-dispersed and retaining their as-synthesized shape and sizes. UV/vis spectroscopic and spectro-electrochemical studies confirmed that the total surface coverage and electrochemically addressable surface coverage of IrO2 NPs increased linearly with the number of bilayers up to 10 bilayers. The voltammetry of the modified electrode was that of hydrous iridium oxide films (HIROFs) with an observed super-Nernstian pH response of the Ir(III)/Ir(IV) and Ir(IV)–Ir(IV)/Ir(IV)–Ir(V) redox transitions and Nernstian shift of the oxygen evolution onset potential. The overpotential of the oxygen evolution reaction (OER) was essentially pH independent, varying only from 0.22 V to 0.28 V (at a current density of 0.1 mA cm 2), moving from acidic to alkaline conditions. Bulk electrolysis experiments revealed that the IrO2/PDDA films were stable and adherent under acidic and neutral conditions but degraded in alkaline solutions. Oxygen was evolved with Faradaic efficiencies approaching 100% under acidic (pH 1) and neutral (pH 7) conditions, and 88% in alkaline solutions (pH 13). This layer-by-layer approach forms the basis of future large-scale OER electrode development using ink-jet printing technology. en_US
dc.language.iso eng en_US
dc.publisher Royal Society of Chemistry en_US
dc.relation 13/SIRG/2137 en_US
dc.relation.ispartofseries Physical Chemistry Chemical Physics;18, pp. 9295-9304
dc.relation.uri http://dx.doi.org/10.1039/C5CP06890H
dc.rights © 2016 Royal Society of Chemistry. Personal use of this material is permitted. Permission from Royal Society of Chemistry must be obtained for all other uses, in any current or future media, including reprinting/republishing this material for advertising or promotional purposes, creating new collective works, for resale or redistribution to servers or lists, or reuse of any copyrighted component of this work in other works en_US
dc.subject Water oxidation en_US
dc.subject IrO2 nanoparticles en_US
dc.subject Electrocatalysis en_US
dc.subject Spectro-electrochemistry en_US
dc.title Boosting water oxidation layer-by-layer 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 2020-01-10T16:28:27Z
dc.description.version ACCEPTED
dc.identifier.doi 10.1039/C5CP06890H
dc.contributor.sponsor SFI en_US
dc.relation.projectid 13/SIRG/2137 en_US
dc.relation.projectid PSPB-35/2010 en_US
dc.rights.accessrights info:eu-repo/semantics/openAccess en_US
dc.internal.rssid 2697081
dc.internal.copyrightchecked Yes
dc.identifier.journaltitle Physical Chemistry Chemical Physics
dc.description.status peer-reviewed


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