TiO2 nanotube arrays decorated with Ir nanoparticles for enhanced hydrogen evolution electrocatalysis
Authors
Lačnjevac, UrošVasilic, 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
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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, applyi...ng 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.
Keywords:
TiO2 nanotube array / acidic electrolyte / galvanic displacement / mass activity / DFT calculationSource:
Programme and the Book of Abstracts / 7th Conference of The Serbian Society for Ceramic Materials, 7CSCS-2023, June 14-16, 2023 Belgrade, Serbia, 2023, 73-74Publisher:
- Belgrade : Institute for Multidisciplinary Research
Funding / projects:
- Development, characterization and application nanostructured and composite electrocatalysts and interactive supports for fuel cells and water electrolysis (RS-MESTD-Basic Research (BR or ON)-172054)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200053 (University of Belgrade, Institute for Multidisciplinary Research) (RS-MESTD-inst-2020-200053)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200146 (University of Belgrade, Faculty of Physical Chemistry) (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)
- ERC
- DFG
- Swedish Research Council, grant agreement No. 2018-05973
- COST action MP1407
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Institution/Community
Institut za multidisciplinarna istraživanjaTY - 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 .