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High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles
dc.creator | Lačnjevac, Uroš | |
dc.creator | Vasilic, Rastko | |
dc.creator | Dobrota, Ana | |
dc.creator | Durdic, Sladana | |
dc.creator | Tomanec, Ondrej | |
dc.creator | Zboril, Radek | |
dc.creator | Mohajernia, Shiva | |
dc.creator | Nhat, Truong Nguyen | |
dc.creator | Skorodumova, Natalia | |
dc.creator | Manojlović, Dragan | |
dc.creator | Elezović, Nevenka R. | |
dc.creator | Pasti, Igor | |
dc.creator | Schmuki, Patrik | |
dc.date.accessioned | 2022-04-05T15:29:58Z | |
dc.date.available | 2022-04-05T15:29:58Z | |
dc.date.issued | 2020 | |
dc.identifier.issn | 2050-7488 | |
dc.identifier.uri | http://rimsi.imsi.bg.ac.rs/handle/123456789/1373 | |
dc.description.abstract | Developing ultraefficient electrocatalytic materials for the hydrogen evolution reaction (HER) with low content of expensive platinum group metals (PGMs) via low-energy-input procedures is the key to the successful commercialization of green water electrolysis technologies for sustainable production of high-purity hydrogen. In this study, we report a facile room-temperature synthesis of ultrafine metallic Ir nanoparticles on conductive, proton-intercalated TiO2 nanotube (H-TNT) arrays via galvanic displacement. A series of experiments demonstrate that a controlled transformation of the H-TNT surface microstructure from neat open-top tubes to disordered nanostripe bundles ("nanograss") is highly beneficial for providing an abundance of exposed Ir active sites. Consequently, for nanograss-engineered composites, outstanding HER activity metrics are achieved even at very low Ir(iii) precursor concentrations. An optimum Ir"TNT cathode loaded with 5.7 mu g(Ir) cm(-2) exhibits an overpotential of -63 mV at -100 mA cm(-2) and a mass activity of 34 A mg(Ir)(-1) at -80 mV under acidic conditions, along with excellent catalytic durability and structural integrity. Density functional theory (DFT) simulations reveal that the hydrogen-rich TiO2 surface not only stabilizes the deposited Ir and weakens its H binding strength to a moderate intensity, but also actively takes part in the HER mechanism by refreshing the Ir catalytic sites near the Ir|H-TiO2 interface, thus substantially promoting H-2 generation. The comprehensive characterization combined with theory provides an in-depth understanding of the electrocatalytic behavior of H-TNT supported PGM nanoparticles and demonstrates their high potential as competitive electrocatalyst systems for the HER. | en |
dc.publisher | Royal Soc Chemistry, Cambridge | |
dc.relation | Republic of Serbia [22] | |
dc.relation | Federal Republic of Germany [22] | |
dc.relation | ERCEuropean Research Council (ERC)European Commission | |
dc.relation | DFGGerman Research Foundation (DFG)European Commission | |
dc.relation | Swedish Research CouncilSwedish Research CouncilEuropean Commission [2018-05973] | |
dc.relation | COST actionEuropean Cooperation in Science and Technology (COST) [MP1407] | |
dc.relation | info:eu-repo/grantAgreement/MESTD/Basic Research (BR or ON)/172054/RS// | |
dc.relation | info:eu-repo/grantAgreement/MESTD/inst-2020/200053/RS// | |
dc.relation | info:eu-repo/grantAgreement/MESTD/inst-2020/200146/RS// | |
dc.rights | restrictedAccess | |
dc.source | Journal of Materials Chemistry A | |
dc.subject | catalyst-support interaction | |
dc.subject | heterostructure | |
dc.subject | DFT calculation | |
dc.subject | hydrogen evolution reaction | |
dc.subject | reaction mechanism | |
dc.title | High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles | en |
dc.type | article | |
dc.rights.license | ARR | |
dc.citation.epage | 22790 | |
dc.citation.issue | 43 | |
dc.citation.other | 8(43): 22773-22790 | |
dc.citation.rank | aM21 | |
dc.citation.spage | 22773 | |
dc.citation.volume | 8 | |
dc.identifier.doi | 10.1039/d0ta07492f | |
dc.identifier.scopus | 2-s2.0-85096105811 | |
dc.identifier.wos | 000589418400026 | |
dc.type.version | publishedVersion |