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Quantitative analysis of the electrochemical performance of multi-redox molecular electrocatalysts. A mechanistic study of chlorate electrocatalytic reduction in presence of a molybdenium polyoxometalate

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dc.contributor.authorGonzález Sánchez, Joaquín
dc.contributor.authorGillén, Esteban
dc.contributor.authorLaborda, Eduardo
dc.contributor.authorMolina, Angela
dc.contributor.departmentQuímica Física
dc.date.accessioned2025-01-20T08:04:55Z
dc.date.available2025-01-20T08:04:55Z
dc.date.issued2022-09
dc.description© 2022 The Authors. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/ This document is the Published Manuscript version of a Published Work that appeared in final form in Journal of Catalysis. To access the final edited and published work see https://doi.org/10.1016/j.jcat.2022.06.038
dc.description.abstractThe quantification of the performance efficiency of a given molecular electrocatalyst versus a particular substrate of interest requires the determination of the rate constants of the catalytic steps taking place in the overall reaction pathway. In this paper, a theoretical model is presented for the quantitative analysis of the voltammetric response of multi-redox catalysts, that is, a molecular species with different redox states that can act in different electrocatalytic forms as a function of the applied potential. The rigorous theoretical model presented incorporates mass transport effects and it is applicable to disc electrodes of any size. As a model system, the electro-reduction of the anion chlorate by the polyoxometalate [PMo12O40]3- (POM) is analysed at gold electrodes. The overall process implies ten charge transfer steps and three different two-electron catalytic processes, the formal potentials and rate constants of which are accurately determined, respectively. The logarithm of the rate constants for the three catalytic steps follows a linear relationship with the average formal potentials of the two-electron charge transfer processes. A comparison with previous efforts devoted to the characterisation of electrocatalytic responses is also carried out, pointing out the advantages of a rigorous solution for this problem.es
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dc.format.extent11es
dc.identifier.citationJournal of Catalysis, 2022, Vol. 413, pp. 467-477
dc.identifier.doihttps://doi.org/10.1016/j.jcat.2022.06.038
dc.identifier.issnPrint: 0021-9517
dc.identifier.issnElectronic: 1090-2694
dc.identifier.urihttp://hdl.handle.net/10201/148801
dc.languageenges
dc.publisherElsevieres
dc.relationFundacion Séneca de la Región de Murcia (Project 19887/GERM/15) y Ministerio de Ciencia e Innovación (PID2019-106097GB-I00/AEI/10.13039/501100011033)es
dc.relation.publisherversionhttps://www.sciencedirect.com/science/article/pii/S0021951722002846es
dc.rightsinfo:eu-repo/semantics/openAccesses
dc.rightsAttribution-NonCommercial-NoDerivatives 4.0 Internacional*
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/*
dc.subject.otherCDU::5 - Ciencias puras y naturales::54 - Química::544 - Química físicaes
dc.titleQuantitative analysis of the electrochemical performance of multi-redox molecular electrocatalysts. A mechanistic study of chlorate electrocatalytic reduction in presence of a molybdenium polyoxometalatees
dc.typeinfo:eu-repo/semantics/articlees
dspace.entity.typePublicationes
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