A simulation and experimental study of electrochemical pH control at gold interdigitated electrode arrays

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dc.check.date2023-08-22
dc.check.infoAccess to this article is restricted until 24 months after publication by request of the publisher.en
dc.contributor.authorO'Sullivan, Benjamin
dc.contributor.authorPatella, Bernardo
dc.contributor.authorDaly, Robert
dc.contributor.authorSeymour, Ian
dc.contributor.authorRobinson, Caoimhe
dc.contributor.authorLovera, Pierre
dc.contributor.authorRohan, James F.
dc.contributor.authorInguanta, Rosalinda
dc.contributor.authorO'Riordan, Alan
dc.contributor.funderIrish Research Councilen
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderDepartment of Agriculture, Food and the Marine, Irelanden
dc.date.accessioned2021-09-17T11:19:28Z
dc.date.available2021-09-17T11:19:28Z
dc.date.issued2021-08-22
dc.date.updated2021-09-16T11:54:15Z
dc.description.abstractIn electroanalysis, solution pH is a critical parameter that often needs to be tailored and controlled for the detection of particular analytes. This is most commonly performed by the addition of chemicals, such as strong acids or bases. Electrochemical in-situ pH control offers the possibility for the local adjustment of pH at the point of detection, without the need for additional reagents. Finite element analysis (FEA) simulations have been performed on interdigitated electrodes, to guide experimental design in relation to both electroanalysis and in-situ control of solution pH. No previous model exists that describes the generation of protons at an interdigitated electrode arrays in solution with one comb acting as a protonator, and the other as the sensor. In this work, FEA models are developed to provide insight into the optimum conditions necessary for electrochemical pH control. The magnitude of applied galvanostatic current has a direct relation to the flux of protons generated and subsequent change in pH. Increasing the separation between the electrodes increases the time taken for protons to diffuse across the gap between the electrode combs. The final pH achieved after 1 second, at both protonator and sensor electrodes, was shown to be largely uninfluenced by a solution's initial pH. The impact of buffer concentration was also modelled and investigated. In practice, the pH at the electrode surface was probed by means of cyclic voltammetry, i.e., to identify the potential of the gold oxide reduction peak. A pH indicator, methyl red, was used to visualise the solution pH change at the electrodes, comparing well with the model's prediction. Finally, we show that in-situ pH controlled detection of mercury in water, using square wave stripping voltammetry, is almost identical to samples acidified to pH 3.5 using nitric acid.en
dc.description.sponsorshipIrish Research Council (Project GOIPG/2015/2925); Science Foundation Ireland (VistaMilk Centre); Department of Agriculture, Food and the Marine, Ireland (Grant Number 16/RC/3835)en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.articleid139113en
dc.identifier.citationO'Sullivan, B., Patella, B., Daly, R., Seymour, I., Robinson, C., Lovera, P., Rohan, J., Inguanta, R. and O'Riordan, A. (2021) 'A simulation and experimental study of electrochemical pH control at gold interdigitated electrode arrays', Electrochimica Acta, 395, 139113 (9pp). doi: 10.1016/j.electacta.2021.139113en
dc.identifier.doi10.1016/j.electacta.2021.139113en
dc.identifier.endpage9en
dc.identifier.issn0013-4686
dc.identifier.journaltitleElectrochimica Actaen
dc.identifier.startpage1en
dc.identifier.urihttps://hdl.handle.net/10468/11946
dc.identifier.volume395en
dc.language.isoenen
dc.publisherElsevier Ltd.en
dc.rights© 2021, Elsevier Ltd. All rights reserved. This manuscript version is made available under the CC BY-NC-ND 4.0 license.en
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectElectroanalysisen
dc.subjectFinite element analysis simulationen
dc.subjectMicroband interdigitated electrode arrayen
dc.subjectSolid state sensorsen
dc.subjectTailored in-situ pH controlen
dc.titleA simulation and experimental study of electrochemical pH control at gold interdigitated electrode arraysen
dc.typeArticle (peer-reviewed)en
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