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dc.creatorBensmann, Boris
dc.creatorPetkovska, Menka
dc.creatorVidaković-Koch, Tanja
dc.creatorHanke-Rauschenbach, Richard
dc.creatorSundmacher, Kai
dc.date.accessioned2021-03-10T11:19:55Z
dc.date.available2021-03-10T11:19:55Z
dc.date.issued2010
dc.identifier.issn0013-4651
dc.identifier.urihttp://TechnoRep.tmf.bg.ac.rs/handle/123456789/1652
dc.description.abstractIn this theoretical contribution, nonlinear frequency response analysis was applied for the investigation of electrochemical methanol oxidation. This technique expresses the input-output behavior of any weakly nonlinear system with the help of the Volterra series expansion and generalized Fourier transform into so-called higher order frequency response functions. These functions contain the system's nonlinear fingerprint. They can be derived analytically from a nonlinear model. These functions can be obtained experimentally from the measurement of higher harmonics induced by a high amplitude sinusoidal perturbation of the system of interest. Frequency response functions up to the second order have been derived analytically for four different model varieties describing the kinetics of the electrochemical methanol oxidation. The first-order frequency response function corresponds to the reciprocal value of the well-known electrochemical impedance, which represents the linear part of the frequency response. This function does not contain sufficient information for discrimination between the different kinetic models. In contrast, the symmetrical second-order frequency response functions H(2)(omega,omega) show differences in shape, which substantiate the availability of the theoretical prerequisites for model discrimination. A detailed parametric study for all four model variants has been performed. The results show that the basic features of the shapes of the H(2)(omega,omega) amplitude spectra corresponding to the four models remain unique. The ubiquitousness of the qualitative differences between the competing models, for the whole set of parameters chosen for our analysis, suggests that the aforementioned amplitude spectra contain sufficient information for an unequivocal model discrimination.en
dc.publisherElectrochemical Soc Inc, Pennington
dc.relationErnest-Solvay-Stiftung
dc.relationinfo:eu-repo/grantAgreement/MESTD/MPN2006-2010/142014/RS//
dc.rightsrestrictedAccess
dc.sourceJournal of the Electrochemical Society
dc.titleNonlinear Frequency Response of Electrochemical Methanol Oxidation Kinetics: A Theoretical Analysisen
dc.typearticle
dc.rights.licenseARR
dc.citation.epageB1289
dc.citation.issue9
dc.citation.other157(9): B1279-B1289
dc.citation.rankaM21
dc.citation.spageB1279
dc.citation.volume157
dc.identifier.doi10.1149/1.3446836
dc.identifier.rcubconv_3433
dc.identifier.scopus2-s2.0-77955794759
dc.identifier.wos000280348300010
dc.type.versionpublishedVersion


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