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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 | Vasilić, Rastko | |
dc.creator | Dobrota, Ana S. | |
dc.creator | Đurđić, Slađana Z. | |
dc.creator | Tomanec, Ondřej | |
dc.creator | Zbořil, Radek | |
dc.creator | Mohajernia, Shiva | |
dc.creator | Nguyen, Nhat Truong | |
dc.creator | Skorodumova, Natalia | |
dc.creator | Manojlović, Dragan D. | |
dc.creator | Elezović, Nevenka | |
dc.creator | Pašti, Igor | |
dc.creator | Schmuki, Patrik | |
dc.date.accessioned | 2020-12-13T19:38:17Z | |
dc.date.available | 2020-12-13T19:38:17Z | |
dc.date.issued | 2020 | |
dc.identifier.issn | 2050-7488 | |
dc.identifier.uri | https://cherry.chem.bg.ac.rs/handle/123456789/4288 | |
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 μgIr cm−2 exhibits an overpotential of −63 mV at −100 mA cm−2 and a mass activity of 34 A mgIr−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 H2 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. | |
dc.language | en | |
dc.publisher | Royal Society of Chemistry | |
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.relation | Bilateral cooperation project between the Republic of Serbia and the Federal Republic of Germany (project years 2020–2021, No. 22), as well as the ERC and DFG. | |
dc.relation | The computations and data handling were enabled by resources provided by the Swedish National Infrastructure for Computing (SNIC) at National Supercomputer Centre (NSC) at Link¨oping University, partially funded by the Swedish Research Council through grant agreement No. 2018-05973. | |
dc.relation | The networking support from COST action MP1407 is greatly appreciated. | |
dc.rights | restrictedAccess | |
dc.source | Journal of Materials Chemistry A | |
dc.title | High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles | |
dc.type | article | en |
dc.rights.license | ARR | |
dcterms.abstract | Нгуyен, Нхат Труонг; Скородумова, Наталиа; Елезовић, Невенка; Пашти, Игор; Сцхмуки, Патрик; Ђурђић, Слађана; Доброта, Aна; Василић, Растко; Лачњевац, Урош; Манојловић, Драган Д.; Томанец, Ондřеј; Збоřил, Радек; Мохајерниа, Схива; | |
dc.citation.volume | 8 | |
dc.citation.issue | 43 | |
dc.citation.spage | 22773 | |
dc.citation.epage | 22790 | |
dc.identifier.wos | 000589418400026 | |
dc.identifier.doi | 10.1039/D0TA07492F | |
dc.citation.rank | M21~ | |
dc.type.version | publishedVersion | |
dc.identifier.scopus | 2-s2.0-85096105811 |