Effective electrocatalytic methanol oxidation of Pd-based metallic glass nanofilms

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dc.authoridIvanov, Yurii/0000-0003-0271-5504
dc.authoridEckert, Jurgen/0000-0003-4112-3181
dc.authoridSarac, Baran/0000-0002-0130-3914
dc.authoridSarac, A.Sezai/0000-0001-7513-1740
dc.authoridPutz, Barbara/0000-0001-9687-6346
dc.authoridGreer, A. Lindsay/0000-0001-7360-5439
dc.contributor.authorSarac, Baran
dc.contributor.authorKarazehir, Tolga
dc.contributor.authorIvanov, Yurii P.
dc.contributor.authorPutz, Barbara
dc.contributor.authorGreer, A. Lindsay
dc.contributor.authorSarac, A. Sezai
dc.contributor.authorEckert, Juergen
dc.date.accessioned2025-01-06T17:44:52Z
dc.date.available2025-01-06T17:44:52Z
dc.date.issued2020
dc.description.abstractCompared to their conventional polycrystalline Pd counterparts, Pd79Au9Si12 (at%) - metallic glass (MG) nanofilm (NF) electrocatalysts offer better methanol oxidation reaction (MOR) in alkaline medium, CO poisoning tolerance and catalyst stability even at high scan rates or high methanol concentrations owing to their amorphous structure without grain boundaries. This study evaluates the influence of scan rate and methanol concentration by cyclic voltammetry, frequency-dependent electrochemical impedance spectroscopy and a related equivalent circuit model at different potentials in Pd-Au-Si amorphous NFs. Structural and compositional differences for the NFs are assessed by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-ray (EDX) mapping and X-ray diffraction (XRD). The ratio of the forward to reverse peak current density i(pf)/i(pb) for the MG NFs is similar to 2.2 times higher than for polycrystalline Pd NFs, evidencing better oxidation of methanol to carbon dioxide in the forward scan and less poisoning of the electrocatalysts by carbonaceous (e.g. CO, HCO) species. Moreover, the electrochemical circuit model obtained from EIS measurements reveals that the MOR occurring around -100 mV increases the capacitance without any significant change in oxidation resistance, whereas CO2 formation towards lower potentials results in a sharp increase in the capacitance of the Faradaic MOR at the catalyst interface and a slight decrease in the corresponding resistance. These results, together with the high i(pf)/i(pb) = 3.37 yielding the minimum amount of carbonaceous species deposited on the thin film during cyclic voltammetry and stability in the alkaline environment, can potentially make these amorphous thin films potential candidates for fuel-cell applications.
dc.description.sponsorshipEuropean Research Council [ERC-2013-ADG-340025, ERC-2015-ADG-695487]; Ministry of Science and Higher Education (Russia) [0657-2020-0005]; Ministry of Science and Higher Education of the Russian Federation [19-13-00207]
dc.description.sponsorshipThe authors thank C. Mitterer and V. Terziyska for providing the sputtering device for synthesizing the MG and Pd NFs. This work was supported by the European Research Council under the Advanced Grants INTELHYB - Next generation of complex metallic materials in intelligent hybrid structures (Grant ERC-2013-ADG-340025) and ExtendGlass - Extending the range of the glassy state: Exploring structure and property limits in metallic glasses (Grant ERC-2015-ADG-695487), and Grant 0657-2020-0005 of the Ministry of Science and Higher Education (Russia), and Ministry of Science and Higher Education of the Russian Federation in the framework of the Increase Competitiveness Program of MISiS (support project for young research engineers, project no. 19-13-00207).
dc.identifier.doi10.1039/d0nr06372j
dc.identifier.endpage22595
dc.identifier.issn2040-3364
dc.identifier.issn2040-3372
dc.identifier.issue44
dc.identifier.pmid33135022
dc.identifier.scopus2-s2.0-85096508596
dc.identifier.scopusqualityQ1
dc.identifier.startpage22586
dc.identifier.urihttps://doi.org/10.1039/d0nr06372j
dc.identifier.urihttps://hdl.handle.net/20.500.14669/3219
dc.identifier.volume12
dc.identifier.wosWOS:000591084100017
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoen
dc.publisherRoyal Soc Chemistry
dc.relation.ispartofNanoscale
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_20241211
dc.subjectAlloy
dc.subjectElectrooxıdatıon
dc.subjectRelaxatıon
dc.subjectNanowıres
dc.subjectStabılıty
dc.subjectPlatınum
dc.subjectEthanol
dc.titleEffective electrocatalytic methanol oxidation of Pd-based metallic glass nanofilms
dc.typeArticle

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