Electrosorption of Hydrogen in Pd-Based Metallic Glass Nanofilms

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dc.authoridEckert, Jurgen/0000-0003-4112-3181
dc.authoridSarac, Baran/0000-0002-0130-3914
dc.authoridSarac, A.Sezai/0000-0001-7513-1740
dc.authoridGammer, Christoph/0000-0003-1917-4978
dc.contributor.authorSarac, Baran
dc.contributor.authorKarazehir, Tolga
dc.contributor.authorMuehlbacher, Marlene
dc.contributor.authorKaynak, Baris
dc.contributor.authorGammer, Christoph
dc.contributor.authorSchoeberl, Thomas
dc.contributor.authorSarac, A. Sezai
dc.date.accessioned2025-01-06T17:44:35Z
dc.date.available2025-01-06T17:44:35Z
dc.date.issued2018
dc.description.abstractAs an efficient potential hydrogen storage and conversion system, hydrogen electrosorption and evolution mechanisms in Pd-based metallic glass thin films (MGTFs) are investigated. In this study, thin films of 55 nm thickness were deposited by dc magnetron sputtering. The amorphous structure of MGTFs and the atomically smooth interface between the MGTF and substrate were confirmed by transmission electron microscopy, whereas the composition-dependent surface roughness was obtained via atomic force microscopy. The shifts in the broad diffraction maxima for the Si and Cu additions were evaluated by X-ray diffraction. The Pd thin film (PdTF) and MGTF working electrodes were chronoamperometrically saturated in 0.5 M H2SO4 solution. The formation of palladium hydride (PdHx) in the MGTFs was investigated by X-ray photoelectron spectroscopy. Cyclic voltammograms were subsequently recorded (between -0.2 and 1.4 V) at sweep rates of 0.02 V s(-1). Electrochemical impedance spectroscopy of MGTFs and PdTF was performed in full spectrum including sorption, desorption, and evolution of hydrogen in a conventional three-electrode configuration. Electrochemical circuit modeling provided the relationship between the composition-dependent hydrogen evolution and H absorption/adsorption processes. The adsorption capacitance parameter Y-ad corresponding to alpha- and beta-hydride formation in the case of Pd0.79Si0.16Cu0.05 MGTF is similar to 5 times higher than that of the crystalline Pd thin film which is in line with the decrease in the charge-transfer resistance R-ct. Addition of Cu disturbs the symmetry of the glass formers, leading to remarkable changes in interfacial hydrogen bonding and diffusion of hydrogen into sublayers. Compared to other Pd-based micron-sized materials, our findings show excellent volumetric hydrogen storage capacity 4 times higher than that of the traditional counterparts of several microns, and 50% higher than the Pd thin films of the same thickness, together with high tunable capacitance, charge-transfer resistance, and diffusivity depending on the glass-forming characteristics of the nanosized MGTF.
dc.description.sponsorshipEuropean Research Council [ERC-2013-ADG-340025]
dc.description.sponsorshipThe authors would like to thank P. Zefferer and A. Rezvan for technical support, C. Mitterer for providing the sputtering device for synthesizing the MGTFs, and Yu. Ivanov, J. Keckes, S. Ketov, and F. Spieckermann for fruitful discussions. This work was supported by the European Research Council under the Advanced Grant INTELHYB-Next Generation of Complex Metallic Materials in Intelligent Hybrid Structures (Grant ERC-2013-ADG-340025).
dc.identifier.doi10.1021/acsaem.8b00330
dc.identifier.endpage2646
dc.identifier.issn2574-0962
dc.identifier.issue6
dc.identifier.scopus2-s2.0-85064731327
dc.identifier.scopusqualityQ1
dc.identifier.startpage2630
dc.identifier.urihttps://doi.org/10.1021/acsaem.8b00330
dc.identifier.urihttps://hdl.handle.net/20.500.14669/3107
dc.identifier.volume1
dc.identifier.wosWOS:000458705800034
dc.identifier.wosqualityN/A
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.language.isoen
dc.publisherAmer Chemical Soc
dc.relation.ispartofAcs Applied Energy Materials
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_20241211
dc.subjectthin films
dc.subjectmetallic glass
dc.subjectpalladium
dc.subjectdc magnetron sputtering
dc.subjectelectrosorption
dc.subjecthydrogen storage and conversion
dc.subjectelectrochemical impedance spectroscopy
dc.subjectcyclic voltammetry
dc.titleElectrosorption of Hydrogen in Pd-Based Metallic Glass Nanofilms
dc.typeArticle

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