Lačnjevac, Uroš

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  • Lačnjevac, Uroš (1)

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High-performance hydrogen evolution electrocatalysis using proton-intercalated TiO2 nanotube arrays as interactive supports for Ir nanoparticles

Lačnjevac, Uroš; Vasilić, Rastko; Dobrota, Ana; Đurđić, Slađana Z.; Tomanec, Ondřej; Zbořil, Radek; Mohajernia, Shiva; Nguyen, Nhat Truong; Skorodumova, Natalia; Manojlović, Dragan D.; Elezović, Nevenka; Pašti, Igor; Schmuki, Patrik

(Royal Society of Chemistry, 2020)

TY  - JOUR
AU  - Lačnjevac, Uroš
AU  - Vasilić, Rastko
AU  - Dobrota, Ana
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  - http://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 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., 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 A, 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, 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 . .
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