High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles
Samo za registrovane korisnike
2020
Autori
Lačnjevac, UrošVasilic, Rastko
Dobrota, Ana
Durdic, Sladana
Tomanec, Ondrej
Zboril, Radek
Mohajernia, Shiva
Nhat, Truong Nguyen
Skorodumova, Natalia
Manojlović, Dragan
Elezović, Nevenka R.
Pasti, Igor
Schmuki, Patrik
Članak u časopisu (Objavljena verzija)
Metapodaci
Prikaz svih podataka o dokumentuApstrakt
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 overpotentia...l 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.
Ključne reči:
catalyst-support interaction / heterostructure / DFT calculation / hydrogen evolution reaction / reaction mechanismIzvor:
Journal of Materials Chemistry A, 2020, 8, 43, 22773-22790Izdavač:
- Royal Soc Chemistry, Cambridge
Finansiranje / projekti:
- Republic of Serbia [22]
- Federal Republic of Germany [22]
- ERCEuropean Research Council (ERC)European Commission
- DFGGerman Research Foundation (DFG)European Commission
- Swedish Research CouncilSwedish Research CouncilEuropean Commission [2018-05973]
- COST actionEuropean Cooperation in Science and Technology (COST) [MP1407]
- Razvoj, karakterizacija i primena nanostruktuiranih kompozitnih katalizatora i interaktivnih nosača u gorivnim spregovima i elektrolizi vode (RS-172054)
- Ministarstvo nauke, tehnološkog razvoja i inovacija Republike Srbije, institucionalno finansiranje - 200053 (Univerzitet u Beogradu, Institut za multidisciplinarna istraživanja) (RS-200053)
- Ministarstvo nauke, tehnološkog razvoja i inovacija Republike Srbije, institucionalno finansiranje - 200146 (Univerzitet u Beogradu, Fakultet za fizičku hemiju) (RS-200146)
DOI: 10.1039/d0ta07492f
ISSN: 2050-7488
WoS: 000589418400026
Scopus: 2-s2.0-85096105811
Institucija/grupa
Institut za multidisciplinarna istraživanjaTY - JOUR AU - Lačnjevac, Uroš AU - Vasilic, Rastko AU - Dobrota, Ana AU - Durdic, Sladana AU - Tomanec, Ondrej AU - Zboril, Radek AU - Mohajernia, Shiva AU - Nhat, Truong Nguyen AU - Skorodumova, Natalia AU - Manojlović, Dragan AU - Elezović, Nevenka R. AU - Pasti, Igor AU - Schmuki, Patrik PY - 2020 UR - http://rimsi.imsi.bg.ac.rs/handle/123456789/1373 AB - 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. PB - Royal Soc Chemistry, Cambridge T2 - Journal of Materials Chemistry A T1 - High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles EP - 22790 IS - 43 SP - 22773 VL - 8 DO - 10.1039/d0ta07492f ER -
@article{ author = "Lačnjevac, Uroš and Vasilic, Rastko and Dobrota, Ana and Durdic, Sladana and Tomanec, Ondrej and Zboril, Radek and Mohajernia, Shiva and Nhat, Truong Nguyen and Skorodumova, Natalia and Manojlović, Dragan and Elezović, Nevenka R. and Pasti, Igor and Schmuki, Patrik", year = "2020", 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.", publisher = "Royal Soc Chemistry, Cambridge", journal = "Journal of Materials Chemistry A", title = "High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles", pages = "22790-22773", number = "43", volume = "8", doi = "10.1039/d0ta07492f" }
Lačnjevac, U., Vasilic, R., Dobrota, A., Durdic, S., Tomanec, O., Zboril, R., Mohajernia, S., Nhat, T. N., Skorodumova, N., Manojlović, D., Elezović, N. R., Pasti, I.,& Schmuki, P.. (2020). High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles. in Journal of Materials Chemistry A Royal Soc Chemistry, Cambridge., 8(43), 22773-22790. https://doi.org/10.1039/d0ta07492f
Lačnjevac U, Vasilic R, Dobrota A, Durdic S, Tomanec O, Zboril R, Mohajernia S, Nhat TN, Skorodumova N, Manojlović D, Elezović NR, Pasti I, Schmuki P. High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles. in Journal of Materials Chemistry A. 2020;8(43):22773-22790. doi:10.1039/d0ta07492f .
Lačnjevac, Uroš, Vasilic, Rastko, Dobrota, Ana, Durdic, Sladana, Tomanec, Ondrej, Zboril, Radek, Mohajernia, Shiva, Nhat, Truong Nguyen, Skorodumova, Natalia, Manojlović, Dragan, Elezović, Nevenka R., Pasti, Igor, Schmuki, Patrik, "High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles" in Journal of Materials Chemistry A, 8, no. 43 (2020):22773-22790, https://doi.org/10.1039/d0ta07492f . .