Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation
Abstract
Heterogeneous catalysts in the form of atomically dispersed metals on a support provide the most efficient utilization of the active component, which is especially important for scarce and expensive late transition metals. These catalysts also enable unique opportunities to understand reaction pathways through detailed spectroscopic and computational studies. Here, we demonstrate that atomically dispersed iridium sites on indium tin oxide prepared via surface organometallic chemistry display exemplary catalytic activity in one of the most challenging electrochemical processes, the oxygen evolution reaction (OER). In situ X-ray absorption studies revealed the formation of IrV=O intermediate under OER conditions with an Ir–O distance of 1.83 Å. Modeling of the reaction mechanism indicates that IrV=O is likely a catalyst resting state, which is subsequently oxidized to IrVI enabling fast water nucleophilic attack and oxygen evolution. We anticipate that the applied strategy can be instrumental in preparing and studying a broad range of atomically dispersed transition metal catalysts on conductive oxides for (photo)electrochemical applications.
- Authors:
-
[1];
[4];
[3];
[5];
[2];
[1]
- Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1-5, CH-8093 Zurich, Switzerland
- Department of Physics and Astronomy, Purdue University, West Lafayette, Indiana 47907, United States
- Departament de Química, Universitat Autònoma de Barcelona, Bellaterra, 08193 Catalonia, Spain
- Scientific Center for Optical and Electron Microscopy (ScopeM), ETH Zurich, Otto-Stern-Weg 3, CH-8093 Zurich, Switzerland
- Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1-5, CH-8093 Zurich, Switzerland, Scientific Center for Optical and Electron Microscopy (ScopeM), ETH Zurich, Otto-Stern-Weg 3, CH-8093 Zurich, Switzerland
- Publication Date:
- Research Org.:
- Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1635568
- Alternate Identifier(s):
- OSTI ID: 1643988
- Grant/Contract Number:
- FG02-10ER16184; AC02-06CH11357
- Resource Type:
- Published Article
- Journal Name:
- ACS Central Science
- Additional Journal Information:
- Journal Name: ACS Central Science Journal Volume: 6 Journal Issue: 7; Journal ID: ISSN 2374-7943
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Radiology; Electrodes; Catalysts; Extended X-ray absorption fine structure; Transition metals
Citation Formats
Lebedev, Dmitry, Ezhov, Roman, Heras-Domingo, Javier, Comas-Vives, Aleix, Kaeffer, Nicolas, Willinger, Marc, Solans-Monfort, Xavier, Huang, Xing, Pushkar, Yulia, and Copéret, Christophe. Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation. United States: N. p., 2020.
Web. doi:10.1021/acscentsci.0c00604.
Lebedev, Dmitry, Ezhov, Roman, Heras-Domingo, Javier, Comas-Vives, Aleix, Kaeffer, Nicolas, Willinger, Marc, Solans-Monfort, Xavier, Huang, Xing, Pushkar, Yulia, & Copéret, Christophe. Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation. United States. https://doi.org/10.1021/acscentsci.0c00604
Lebedev, Dmitry, Ezhov, Roman, Heras-Domingo, Javier, Comas-Vives, Aleix, Kaeffer, Nicolas, Willinger, Marc, Solans-Monfort, Xavier, Huang, Xing, Pushkar, Yulia, and Copéret, Christophe. Wed .
"Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation". United States. https://doi.org/10.1021/acscentsci.0c00604.
@article{osti_1635568,
title = {Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation},
author = {Lebedev, Dmitry and Ezhov, Roman and Heras-Domingo, Javier and Comas-Vives, Aleix and Kaeffer, Nicolas and Willinger, Marc and Solans-Monfort, Xavier and Huang, Xing and Pushkar, Yulia and Copéret, Christophe},
abstractNote = {Heterogeneous catalysts in the form of atomically dispersed metals on a support provide the most efficient utilization of the active component, which is especially important for scarce and expensive late transition metals. These catalysts also enable unique opportunities to understand reaction pathways through detailed spectroscopic and computational studies. Here, we demonstrate that atomically dispersed iridium sites on indium tin oxide prepared via surface organometallic chemistry display exemplary catalytic activity in one of the most challenging electrochemical processes, the oxygen evolution reaction (OER). In situ X-ray absorption studies revealed the formation of IrV=O intermediate under OER conditions with an Ir–O distance of 1.83 Å. Modeling of the reaction mechanism indicates that IrV=O is likely a catalyst resting state, which is subsequently oxidized to IrVI enabling fast water nucleophilic attack and oxygen evolution. We anticipate that the applied strategy can be instrumental in preparing and studying a broad range of atomically dispersed transition metal catalysts on conductive oxides for (photo)electrochemical applications.},
doi = {10.1021/acscentsci.0c00604},
journal = {ACS Central Science},
number = 7,
volume = 6,
place = {United States},
year = {Wed Jul 01 00:00:00 EDT 2020},
month = {Wed Jul 01 00:00:00 EDT 2020}
}
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