The role of reactive reaction intermediates in two-step heterogeneous electro-catalytic reactions: a model study
dc.bibliographicCitation.seriesTitle | WIAS Preprints | eng |
dc.bibliographicCitation.volume | 1522 | |
dc.contributor.author | Fuhrmann, Jürgen | |
dc.contributor.author | Zhao, H. | |
dc.contributor.author | Langmach, H. | |
dc.contributor.author | Seidel, Y.E. | |
dc.contributor.author | Jusys, Z. | |
dc.contributor.author | Behm, R.J. | |
dc.date.accessioned | 2016-03-24T17:38:38Z | |
dc.date.available | 2019-06-28T08:05:38Z | |
dc.date.issued | 2010 | |
dc.description.abstract | Experimental investigations of heterogeneous electrocatalytic reactions have been performed in flow cells which provide an environment with controlled parameters. Measurements of the oxygen reduction reaction in a flow cell with an electrode consisting of an array of Pt nanodisks on a glassy carbon substrate exhibited a decreasing fraction of the intermediate $H_2O_2$ in the overall reaction products with increasing density of the nanodiscs. A similar result is true for the dependence on the catalyst loading in the case of a supported Pt/C catalyst thin-film electrode, where the fraction of the intermediate decreases with increasing catalyst loading. Similar effects have been detected for the methanol oxidation. We present a model of multistep heterogeneous electrocatalytic oxidation and reduction reactions based on an adsorption-reaction-desorption scheme using the Langmuir assumption and macroscopic transport equations. A continuum based model problem in a vertical cross section of a rectangular flow cell is proposed in order to explain basic principles of the experimental situation. It includes three model species A, B, C, which undergo adsorption and desorption at a catalyst surface, as well as adsorbate reactions from A to B to C. These surface reactions are coupled with diffusion and advection in the Hagen Poiseuille flow in the flow chamber of the cell. Both high velocity asymptotic theory and a finite volume numerical are used to obtain approximate solutions to the model. Both approaches show a behaviour similar to the experimentally observed. Working in more general situations, the finite volume scheme was applied to a catalyst layer consisting of a number of small catalytically active areas corresponding to nanodisks. Good qualitative agreement with the experimental findings was established for this case as well. | eng |
dc.description.version | publishedVersion | eng |
dc.format | application/pdf | |
dc.identifier.issn | 0946-8633 | |
dc.identifier.uri | https://doi.org/10.34657/3365 | |
dc.identifier.uri | https://oa.tib.eu/renate/handle/123456789/2327 | |
dc.language.iso | eng | eng |
dc.publisher | Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik | eng |
dc.relation.issn | 0946-8633 | eng |
dc.rights.license | This document may be downloaded, read, stored and printed for your own use within the limits of § 53 UrhG but it may not be distributed via the internet or passed on to external parties. | eng |
dc.rights.license | Dieses Dokument darf im Rahmen von § 53 UrhG zum eigenen Gebrauch kostenfrei heruntergeladen, gelesen, gespeichert und ausgedruckt, aber nicht im Internet bereitgestellt oder an Außenstehende weitergegeben werden. | ger |
dc.subject.ddc | 510 | eng |
dc.subject.other | Finite volume method | eng |
dc.subject.other | electrocatalysis | eng |
dc.title | The role of reactive reaction intermediates in two-step heterogeneous electro-catalytic reactions: a model study | eng |
dc.type | Report | eng |
dc.type | Text | eng |
tib.accessRights | openAccess | eng |
wgl.contributor | WIAS | eng |
wgl.subject | Mathematik | eng |
wgl.type | Report / Forschungsbericht / Arbeitspapier | eng |
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