TY  - CONF
AU  - Lačnjevac, Uroš
AU  - Vasilic, Rastko
AU  - Dobrota, Ana S.
AU  - Đurđić, Slađana
AU  - Tomanec, Ondřej
AU  - Zbořil, Radek
AU  - Mohajernia, Shiva
AU  - Nguyen, Nhat Truong
AU  - Skorodumova, Natalia
AU  - Manojlović, Dragan
AU  - Elezović, Nevenka R.
AU  - Pasti, Igor
AU  - Schmuki, Patrik
PY  - 2023
UR  - http://rimsi.imsi.bg.ac.rs/handle/123456789/2843
AB  - Designing cost-effective hydrogen evolution reaction (HER) electrocatalysts containing highly active, but expensive platinum group metals (PGMs) is key to the commercialization of polymer electrolyte membrane water electrolysis systems for green hydrogen production. Our recent investigations have shown that efficient and durable HER composite cathodes can be prepared by spontaneous deposition of PGM nanoparticles on self-aligned titania nanotube (TNT) arrays formed by anodization [1]. In this synthesis route, anatase TNTs are first cathodically protonated (H-TNT), and then used as the reducing agent for PGM ions at room temperature. Herein, we employ the galvanic displacement strategy to decorate H-TNT arrays with ultrafine Ir nanoparticles [2]. We demonstrate that transforming the top surface morphology of supporting TNT arrays from ordered open-top tubes to bundled nanowires (“nanograss”) is beneficial for exposing more Ir active centers during the HER operation. Consequently, applying very low concentrations of Ir(III) ions in the galvanic displacement step is sufficient to produce exceptionally active nanograss-modified Ir@TNT composites. An optimum Ir@TNT, possessing a low Ir loading of 5.7 μgIr cm–2, requires an overpotential of only –63 mV to reach a current density of –100 mA cm–2 and shows a stable long-term performance in a 1 M HClO4 solution. Computational simulations suggest that the hydrogen-rich TiO2 support not only strongly interacts with anchored Ir particles and weakens their H binding strength to a moderate level, but also actively provides hydrogen for rejuvenation of the Ir active sites at the Ir|H-TiO2 interface, thereby significantly enhancing HER catalysis.

[1] U.Č. Lačnjevac, R. Vasilić, T. Tokarski, G. Cios, P. Żabiński, N. Elezović and N. V. Krstajić, Nano Energy 47 (2018) 527.
[2] U. Lačnjevac, R. Vasilić, A. Dobrota, S. Đurđić, O. Tomanec, R. Zbořil, S. Mohajernia, N.T. Nguyen, N. Skorodumova, D. Manojlović, N. Elezović, I. Pašti, P. Schmuki, Journal of Materials Chemistry A 8 (2020) 22773.
PB  - Belgrade : Institute for Multidisciplinary Research
C3  - Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia
T1  - TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis
EP  - 74
SP  - 73
UR  - https://hdl.handle.net/21.15107/rcub_rimsi_2843
ER  - 

@conference{
author = "Lačnjevac, Uroš and Vasilic, Rastko and Dobrota, Ana S. and Đurđić, Slađana and Tomanec, Ondřej and Zbořil, Radek and Mohajernia, Shiva and Nguyen, Nhat Truong and Skorodumova, Natalia and Manojlović, Dragan and Elezović, Nevenka R. and Pasti, Igor and Schmuki, Patrik",
year = "2023",
abstract = "Designing cost-effective hydrogen evolution reaction (HER) electrocatalysts containing highly active, but expensive platinum group metals (PGMs) is key to the commercialization of polymer electrolyte membrane water electrolysis systems for green hydrogen production. Our recent investigations have shown that efficient and durable HER composite cathodes can be prepared by spontaneous deposition of PGM nanoparticles on self-aligned titania nanotube (TNT) arrays formed by anodization [1]. In this synthesis route, anatase TNTs are first cathodically protonated (H-TNT), and then used as the reducing agent for PGM ions at room temperature. Herein, we employ the galvanic displacement strategy to decorate H-TNT arrays with ultrafine Ir nanoparticles [2]. We demonstrate that transforming the top surface morphology of supporting TNT arrays from ordered open-top tubes to bundled nanowires (“nanograss”) is beneficial for exposing more Ir active centers during the HER operation. Consequently, applying very low concentrations of Ir(III) ions in the galvanic displacement step is sufficient to produce exceptionally active nanograss-modified Ir@TNT composites. An optimum Ir@TNT, possessing a low Ir loading of 5.7 μgIr cm–2, requires an overpotential of only –63 mV to reach a current density of –100 mA cm–2 and shows a stable long-term performance in a 1 M HClO4 solution. Computational simulations suggest that the hydrogen-rich TiO2 support not only strongly interacts with anchored Ir particles and weakens their H binding strength to a moderate level, but also actively provides hydrogen for rejuvenation of the Ir active sites at the Ir|H-TiO2 interface, thereby significantly enhancing HER catalysis.

[1] U.Č. Lačnjevac, R. Vasilić, T. Tokarski, G. Cios, P. Żabiński, N. Elezović and N. V. Krstajić, Nano Energy 47 (2018) 527.
[2] U. Lačnjevac, R. Vasilić, A. Dobrota, S. Đurđić, O. Tomanec, R. Zbořil, S. Mohajernia, N.T. Nguyen, N. Skorodumova, D. Manojlović, N. Elezović, I. Pašti, P. Schmuki, Journal of Materials Chemistry A 8 (2020) 22773.",
publisher = "Belgrade : Institute for Multidisciplinary Research",
journal = "Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia",
title = "TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis",
pages = "74-73",
url = "https://hdl.handle.net/21.15107/rcub_rimsi_2843"
}

Lačnjevac, U., Vasilic, R., Dobrota, A. S., Đurđić, S., Tomanec, O., Zbořil, R., Mohajernia, S., Nguyen, N. T., Skorodumova, N., Manojlović, D., Elezović, N. R., Pasti, I.,& Schmuki, P.. (2023). TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis. in Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia
Belgrade : Institute for Multidisciplinary Research., 73-74.
https://hdl.handle.net/21.15107/rcub_rimsi_2843

Lačnjevac U, Vasilic R, Dobrota AS, Đurđić S, Tomanec O, Zbořil R, Mohajernia S, Nguyen NT, Skorodumova N, Manojlović D, Elezović NR, Pasti I, Schmuki P. TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis. in Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia. 2023;:73-74.
https://hdl.handle.net/21.15107/rcub_rimsi_2843 .

Lačnjevac, Uroš, Vasilic, Rastko, Dobrota, Ana S., Đurđić, Slađana, Tomanec, Ondřej, Zbořil, Radek, Mohajernia, Shiva, Nguyen, Nhat Truong, Skorodumova, Natalia, Manojlović, Dragan, Elezović, Nevenka R., Pasti, Igor, Schmuki, Patrik, "TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis" in Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia (2023):73-74,
https://hdl.handle.net/21.15107/rcub_rimsi_2843 .

TY  - 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 . .

TY  - CONF
AU  - Ribić, Vesna
AU  - Dapčević, Aleksandra
AU  - Skorodumova, Natalia
AU  - Rečnik, Aleksander
AU  - Luković Golić, Danijela
AU  - Branković, Goran
PY  - 2018
UR  - http://rimsi.imsi.bg.ac.rs/handle/123456789/2404
PB  - epcc, Edinburgh, UK
C3  - HPC–Europa Transnational Access Meeting (TAM 2018)
T1  - DFT screening of Gd as a dopant in the BiFeO3 superlattice
UR  - https://hdl.handle.net/21.15107/rcub_rimsi_2404
ER  - 

@conference{
author = "Ribić, Vesna and Dapčević, Aleksandra and Skorodumova, Natalia and Rečnik, Aleksander and Luković Golić, Danijela and Branković, Goran",
year = "2018",
publisher = "epcc, Edinburgh, UK",
journal = "HPC–Europa Transnational Access Meeting (TAM 2018)",
title = "DFT screening of Gd as a dopant in the BiFeO3 superlattice",
url = "https://hdl.handle.net/21.15107/rcub_rimsi_2404"
}

Ribić, V., Dapčević, A., Skorodumova, N., Rečnik, A., Luković Golić, D.,& Branković, G.. (2018). DFT screening of Gd as a dopant in the BiFeO3 superlattice. in HPC–Europa Transnational Access Meeting (TAM 2018)
epcc, Edinburgh, UK..
https://hdl.handle.net/21.15107/rcub_rimsi_2404

Ribić V, Dapčević A, Skorodumova N, Rečnik A, Luković Golić D, Branković G. DFT screening of Gd as a dopant in the BiFeO3 superlattice. in HPC–Europa Transnational Access Meeting (TAM 2018). 2018;.
https://hdl.handle.net/21.15107/rcub_rimsi_2404 .

Ribić, Vesna, Dapčević, Aleksandra, Skorodumova, Natalia, Rečnik, Aleksander, Luković Golić, Danijela, Branković, Goran, "DFT screening of Gd as a dopant in the BiFeO3 superlattice" in HPC–Europa Transnational Access Meeting (TAM 2018) (2018),
https://hdl.handle.net/21.15107/rcub_rimsi_2404 .

TY  - CONF
AU  - Ribić, Vesna
AU  - Dapčević, Aleksandra
AU  - Skorodumova, Natalia
AU  - Rečnik, Aleksander
AU  - Luković Golić, Danijela
AU  - Branković, Zorica
AU  - Branković, Goran
PY  - 2018
UR  - http://rimsi.imsi.bg.ac.rs/handle/123456789/2394
PB  - HPC-Europa3, Ljubljana, Slovenija
C3  - European HPC Summit Week 2018 – #EHPCSW
T1  - First-Principles Calculation of Gd - doped BiFeO3
SP  - 28
UR  - https://hdl.handle.net/21.15107/rcub_rimsi_2394
ER  - 

@conference{
author = "Ribić, Vesna and Dapčević, Aleksandra and Skorodumova, Natalia and Rečnik, Aleksander and Luković Golić, Danijela and Branković, Zorica and Branković, Goran",
year = "2018",
publisher = "HPC-Europa3, Ljubljana, Slovenija",
journal = "European HPC Summit Week 2018 – #EHPCSW",
title = "First-Principles Calculation of Gd - doped BiFeO3",
pages = "28",
url = "https://hdl.handle.net/21.15107/rcub_rimsi_2394"
}

Ribić, V., Dapčević, A., Skorodumova, N., Rečnik, A., Luković Golić, D., Branković, Z.,& Branković, G.. (2018). First-Principles Calculation of Gd - doped BiFeO3. in European HPC Summit Week 2018 – #EHPCSW
HPC-Europa3, Ljubljana, Slovenija., 28.
https://hdl.handle.net/21.15107/rcub_rimsi_2394

Ribić V, Dapčević A, Skorodumova N, Rečnik A, Luković Golić D, Branković Z, Branković G. First-Principles Calculation of Gd - doped BiFeO3. in European HPC Summit Week 2018 – #EHPCSW. 2018;:28.
https://hdl.handle.net/21.15107/rcub_rimsi_2394 .

Ribić, Vesna, Dapčević, Aleksandra, Skorodumova, Natalia, Rečnik, Aleksander, Luković Golić, Danijela, Branković, Zorica, Branković, Goran, "First-Principles Calculation of Gd - doped BiFeO3" in European HPC Summit Week 2018 – #EHPCSW (2018):28,
https://hdl.handle.net/21.15107/rcub_rimsi_2394 .