Ethanol electro-oxidation in an alkaline medium using Pd/C, Au/C and PdAu/C electrocatalysts prepared by electron beam irradiation

dc.contributorUniversidade Estadual Paulista (UNESP)
dc.creatorGeraldes, Adriana Napoleão
dc.creatorDa Silva, Dionisio Furtunato
dc.creatorPino, Eddy Segura
dc.creatorDa Silva, Júlio César Martins
dc.creatorDe Souza, Rodrigo Fernando Brambilla
dc.creatorHammer, Peter
dc.creatorSpinacé, Estevam Vitório
dc.creatorNeto, Almir Oliveira
dc.creatorLinardi, Marcelo
dc.creatorDos Santos, Mauro Coelho
dc.date2014-05-27T11:30:41Z
dc.date2016-10-25T18:54:06Z
dc.date2014-05-27T11:30:41Z
dc.date2016-10-25T18:54:06Z
dc.date2013-09-11
dc.date.accessioned2017-04-06T02:38:50Z
dc.date.available2017-04-06T02:38:50Z
dc.identifierElectrochimica Acta, v. 111, p. 455-465.
dc.identifier0013-4686
dc.identifierhttp://hdl.handle.net/11449/76545
dc.identifierhttp://acervodigital.unesp.br/handle/11449/76545
dc.identifier10.1016/j.electacta.2013.08.021
dc.identifierWOS:000329531100061
dc.identifier2-s2.0-84883524606
dc.identifierhttp://dx.doi.org/10.1016/j.electacta.2013.08.021
dc.identifier.urihttp://repositorioslatinoamericanos.uchile.cl/handle/2250/897238
dc.descriptionCarbon-supported Pd, Au and bimetallic PdAu (Pd:Au 90:10, 50:50 and 30:70 atomic ratios) electrocatalysts were prepared using electron beam irradiation. The obtained materials were characterized by energy dispersive X-ray analysis (EDX), X-ray diffraction (XRD) and transmission electron microscopy (TEM), and their catalytic activities toward ethanol electro-oxidation were evaluated in an alkaline medium using electrochemical techniques, in situ attenuated total reflectance Fourier transformed infrared spectroscopy (ATR-FTIR) analysis and a single alkaline direct ethanol fuel cell (ADEFC). EDX analyses showed that the actual Pd: Au atomic ratios were very similar to the nominal ones. X-ray diffractograms of PdAu/C electrocatalysts evidenced the presence of Pd-rich (fcc) and Au-rich (fcc) phases. TEM analysis showed a homogeneous dispersion of nanoparticles on the carbon support, with an average size in the range of 3-5 nm and broad size distributions. Cyclic voltammetry (CV) and chronoamperometry (CA) experiments revealed the superior ambient activity toward ethanol electro-oxidation of PdAu/C electrocatalysts with Pd: Au ratios of 90:10 and 50:50. In situ ATR-FTIR spectroscopy measurements have shown that the mechanism for ethanol electro-oxidation is dependent on catalyst composition, leading to different reaction products, such as acetaldehyde and acetate, depending on the number of electrons transferred. Experiments on a single ADEFC were conducted between 50 and 900 C, and the best performance of 44 mW cm-2 in 2.0molL-1 ethanol was obtained at 850C for the Pd:Au 90:10 catalysts. This superior performance is most likely associated with enhancement of ethanol adsorption on Pd, oxidation of the intermediates, the presence of gold oxide-hydroxyl species, low mean particle diameters and better distribution of particles on the support. © 2013 Elsevier Ltd. All rights reserved.
dc.languageeng
dc.relationElectrochimica Acta
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.subjectAlkaline direct ethanol fuel cell
dc.subjectDAAFC
dc.subjectElectron beam irradiation
dc.subjectEthanol electro-oxidation
dc.subjectFuel cell
dc.subjectPdAu/C
dc.subjectAttenuated total reflectance
dc.subjectElectrochemical techniques
dc.subjectEnergy dispersive x-ray analysis (EDX)
dc.subjectFourier transformed infrared spectroscopy
dc.subjectCarbon
dc.subjectCatalyst activity
dc.subjectChronoamperometry
dc.subjectCyclic voltammetry
dc.subjectDirect ethanol fuel cells (DEFC)
dc.subjectElectrocatalysts
dc.subjectElectrolysis
dc.subjectElectron beams
dc.subjectElectrooxidation
dc.subjectEthanol
dc.subjectExperiments
dc.subjectFourier transform infrared spectroscopy
dc.subjectFuel cells
dc.subjectIrradiation
dc.subjectReaction intermediates
dc.subjectTransmission electron microscopy
dc.subjectX ray diffraction
dc.subjectPalladium
dc.titleEthanol electro-oxidation in an alkaline medium using Pd/C, Au/C and PdAu/C electrocatalysts prepared by electron beam irradiation
dc.typeOtro


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