The origin of the high electrochemical activity of pseudo-amorphous iridium oxides

Marine Elmaalouf, Mateusz Odziomek, Silvia Duran, Maxime Gayrard, Mounib Bahri, Cédric Tard, Andrea Zitolo, Benedikt Lassalle-Kaiser, Jean-Yves Piquemal, Ovidiu Ersen, Cédric Boissière, Clément Sanchez, Marion Giraud (), Marco Faustini () and Jennifer Peron ()
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Marine Elmaalouf: ITODYS, CNRS, UMR 7086, Université de Paris
Mateusz Odziomek: Sorbonne Université, CNRS, Collège de France, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, UMR 7574
Silvia Duran: Laboratoire de Chimie Moléculaire (LCM), CNRS, Ecole Polytechnique, Institut Polytechnique de Paris
Maxime Gayrard: Sorbonne Université, CNRS, Collège de France, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, UMR 7574
Mounib Bahri: IPCMS, CNRS, Université de Strasbourg
Cédric Tard: Laboratoire de Chimie Moléculaire (LCM), CNRS, Ecole Polytechnique, Institut Polytechnique de Paris
Andrea Zitolo: Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin
Benedikt Lassalle-Kaiser: Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin
Jean-Yves Piquemal: ITODYS, CNRS, UMR 7086, Université de Paris
Ovidiu Ersen: IPCMS, CNRS, Université de Strasbourg
Cédric Boissière: Sorbonne Université, CNRS, Collège de France, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, UMR 7574
Clément Sanchez: Sorbonne Université, CNRS, Collège de France, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, UMR 7574
Marion Giraud: ITODYS, CNRS, UMR 7086, Université de Paris
Marco Faustini: Sorbonne Université, CNRS, Collège de France, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, UMR 7574
Jennifer Peron: ITODYS, CNRS, UMR 7086, Université de Paris

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Combining high activity and stability, iridium oxide remains the gold standard material for the oxygen evolution reaction in acidic medium for green hydrogen production. The reasons for the higher electroactivity of amorphous iridium oxides compared to their crystalline counterpart is still the matter of an intense debate in the literature and, a comprehensive understanding is needed to optimize its use and allow for the development of water electrolysis. By producing iridium-based mixed oxides using aerosol, we are able to decouple the electronic processes from the structural transformation, i.e. Ir oxidation from IrO2 crystallization, occurring upon calcination. Full characterization using in situ and ex situ X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and transmission electron microscopy allows to unambiguously attribute their high electrochemical activity to structural features and rules out the iridium oxidation state as a critical parameter. This study indicates that short-range ordering, corresponding to sub-2nm crystal size for our samples, drives the activity independently of the initial oxidation state and composition of the calcined iridium oxides.

Date: 2021
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DOI: 10.1038/s41467-021-24181-x

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