High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles
Samo za registrovane korisnike
2020
Autori
Lačnjevac, UrošVasilić, Rastko
Dobrota, Ana S.
Đurđić, Slađana Z.
Tomanec, Ondřej
Zbořil, Radek
Mohajernia, Shiva
Nguyen, Nhat Truong
Skorodumova, Natalia
Manojlović, Dragan D.
Elezović, Nevenka
Pašti, 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 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.
Izvor:
Journal of Materials Chemistry A, 2020, 8, 43, 22773-22790Izdavač:
- Royal Society of Chemistry
Finansiranje / projekti:
- Razvoj, karakterizacija i primena nanostruktuiranih kompozitnih katalizatora i interaktivnih nosača u gorivnim spregovima i elektrolizi vode (RS-MESTD-Basic Research (BR or ON)-172054)
- Ministarstvo nauke, tehnološkog razvoja i inovacija Republike Srbije, institucionalno finansiranje - 200053 (Univerzitet u Beogradu, Institut za multidisciplinarna istraživanja) (RS-MESTD-inst-2020-200053)
- Ministarstvo nauke, tehnološkog razvoja i inovacija Republike Srbije, institucionalno finansiranje - 200146 (Univerzitet u Beogradu, Fakultet za fizičku hemiju) (RS-MESTD-inst-2020-200146)
- 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.
- 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.
- The networking support from COST action MP1407 is greatly appreciated.
DOI: 10.1039/D0TA07492F
ISSN: 2050-7488
WoS: 000589418400026
Scopus: 2-s2.0-85096105811
Kolekcije
Institucija/grupa
Hemijski fakultet / Faculty of ChemistryTY - JOUR AU - Lačnjevac, Uroš AU - Vasilić, Rastko AU - Dobrota, Ana S. AU - Đurđić, Slađana Z. AU - Tomanec, Ondřej AU - Zbořil, Radek AU - Mohajernia, Shiva AU - Nguyen, Nhat Truong AU - Skorodumova, Natalia AU - Manojlović, Dragan D. AU - Elezović, Nevenka AU - Pašti, Igor AU - Schmuki, Patrik PY - 2020 UR - https://cherry.chem.bg.ac.rs/handle/123456789/4288 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 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. PB - Royal Society of Chemistry T2 - Journal of Materials Chemistry A T1 - High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles VL - 8 IS - 43 SP - 22773 EP - 22790 DO - 10.1039/D0TA07492F ER -
@article{ author = "Lačnjevac, Uroš and Vasilić, Rastko and Dobrota, Ana S. and Đurđić, Slađana Z. and Tomanec, Ondřej and Zbořil, Radek and Mohajernia, Shiva and Nguyen, Nhat Truong and Skorodumova, Natalia and Manojlović, Dragan D. and Elezović, Nevenka and Pašti, 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 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.", publisher = "Royal Society of Chemistry", journal = "Journal of Materials Chemistry A", title = "High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles", volume = "8", number = "43", pages = "22773-22790", doi = "10.1039/D0TA07492F" }
Lačnjevac, U., Vasilić, R., Dobrota, A. S., Đurđić, S. Z., Tomanec, O., Zbořil, R., Mohajernia, S., Nguyen, N. T., Skorodumova, N., Manojlović, D. D., Elezović, N., Pašti, 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 Society of Chemistry., 8(43), 22773-22790. https://doi.org/10.1039/D0TA07492F
Lačnjevac U, Vasilić R, Dobrota AS, Đurđić SZ, Tomanec O, Zbořil R, Mohajernia S, Nguyen NT, Skorodumova N, Manojlović DD, Elezović N, Pašti 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, Vasilić, Rastko, Dobrota, Ana S., Đurđić, Slađana Z., Tomanec, Ondřej, Zbořil, Radek, Mohajernia, Shiva, Nguyen, Nhat Truong, Skorodumova, Natalia, Manojlović, Dragan D., Elezović, Nevenka, Pašti, 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 . .