Synergistic enhancement of hydrogen interactions in palladium-silicon-gold metallic glass with multilayered graphene

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dc.authoridMitterer, Christian/0000-0002-7768-7926
dc.authoridSarac, A.Sezai/0000-0001-7513-1740
dc.authoridGreer, A. Lindsay/0000-0001-7360-5439
dc.authoridEckert, Jurgen/0000-0003-4112-3181
dc.authoridPutz, Barbara/0000-0001-9687-6346
dc.contributor.authorSarac, Baran
dc.contributor.authorIvanov, Yurii P.
dc.contributor.authorPutz, Barbara
dc.contributor.authorKarazehir, Tolga
dc.contributor.authorMitterer, Christian
dc.contributor.authorGreer, A. Lindsay
dc.contributor.authorSarac, A. Sezai
dc.date.accessioned2025-01-06T17:44:57Z
dc.date.available2025-01-06T17:44:57Z
dc.date.issued2023
dc.description.abstractAmorphous PdSiAu-based metallic glass thin films (MGTFs) obtained by physical vapor deposition were deposited on multilayered graphene (MLGR) supported on Si/SiO2, where the MLGR is carried to the top by upward pressure of the deposited atomic layer passing through the crystal lattice of graphene. Samples were electrochemically hydrogenated by chronoamperometry and characterized by cyclic voltammetry in 0.1 M H2SO4. MLGR-containing samples have a prominent Raman peak at 1415 cm-1. This sample shows & SIM;2.6 times larger hydrogen desorption charge and & SIM;4.5 times larger electrocatalytic hydrogen activity compared to the MLGR-free counterparts. Furthermore, the capacitance retrieved from the simulation of electrochemical impedance data indicates a & SIM;2.6 times increase upon MLGR inclusion. High-resolution (scanning) transmission electron microscopy after hydrogenation corroborates the existence of nm-sized PdHx crystals around the MGTF-Si/SiO2 interface and the presence of a graphene layer on top of the MGTF due to bond breaking between the MLGR and Si/SiO2. The enhanced hydrogen activity due to the synergistic effect of MLGR and MGTF layer-by-layer nanostructure reveals itself in the diffusion kinetics, where 50% faster hydrogen ion transfer into the MGTF is obtained when the MLGR top layer is present. The areal and volumetric hydrogen desorption charge exceed almost all the considered Pd-based counterparts, especially when comparing systems with similar thicknesses. Hence, the developed hybrid nanostructure can be envisaged as an alternative ultra-high hydrogen charger for small-scale applications. Presence of only a few layers of graphene boosts hydrogen intake of Pd-based metallic glass thin films by 2.6 times with 4.5 times higher electrocatalytic hydrogen evolution reaction activity, a tremendous improvement in metal-hydrogen interactions.
dc.description.sponsorshipThe authors thank V. Terziyska for assistance with synthesizing the nanofilms and M. Aydin for support with Raman spectroscopy. This work was supported by the European Research Council under the Advanced Grant INTELHYB - Next generation of complex metalli
dc.description.sponsorshipThe authors thank V. Terziyska for assistance with synthesizing the nanofilms and M. Aydin for support with Raman spectroscopy. 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), ExtendGlass - Extending the range of the glassy state: exploring structure and property limits in metallic glasses (Grant ERC-2015-ADG-695487), and the Austrian Science Fund (FWF) under project grant I3937-N36.
dc.identifier.doi10.1039/d3ta01734f
dc.identifier.endpage19407
dc.identifier.issn2050-7488
dc.identifier.issn2050-7496
dc.identifier.issue36
dc.identifier.scopus2-s2.0-85170693404
dc.identifier.scopusqualityQ1
dc.identifier.startpage19396
dc.identifier.urihttps://doi.org/10.1039/d3ta01734f
dc.identifier.urihttps://hdl.handle.net/20.500.14669/3256
dc.identifier.volume11
dc.identifier.wosWOS:001055809500001
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.language.isoen
dc.publisherRoyal Soc Chemistry
dc.relation.ispartofJournal of Materials Chemistry A
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_20241211
dc.subjectEvolutıon Reactıon
dc.subjectHıghly Effıcıent
dc.subjectThın-Fılms
dc.subjectPd
dc.subjectAdsorptıon
dc.subjectStorage
dc.subjectBehavıor
dc.subjectElectrodes
dc.subjectAlloys
dc.subjectNanopartıcles
dc.titleSynergistic enhancement of hydrogen interactions in palladium-silicon-gold metallic glass with multilayered graphene
dc.typeArticle

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