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DOI10.1039/c9ee01872g
Degradation of iridium oxides via oxygen evolution from the lattice: Correlating atomic scale structure with reaction mechanisms
Kasian O.; Geiger S.; Li T.; Grote J.-P.; Schweinar K.; Zhang S.; Scheu C.; Raabe D.; Cherevko S.; Gault B.; Mayrhofer K.J.J.
发表日期2019
ISSN1754-5692
起始页码3548
结束页码3555
卷号12期号:12
英文摘要Understanding the fundamentals of iridium degradation during the oxygen evolution reaction is of importance for the development of efficient and durable water electrolysis systems. The degradation mechanism is complex and it is under intense discussion whether the oxygen molecule can be directly released from the oxide lattice. Here, we define the extent of lattice oxygen participation in the oxygen evolution and associated degradation of rutile and hydrous iridium oxide catalysts, and correlate this mechanism with the atomic-scale structures of the catalytic surfaces. We combine isotope labelling with atom probe tomography, online electrochemical and inductively coupled plasma mass spectrometry. Our data reveal that, unlike rutile IrO2, Ir hydrous oxide contains -IrIIIOOH species which directly contribute to the oxygen evolution from the lattice. This oxygen evolution mechanism results in faster degradation and dissolution of Ir. In addition, near surface bulk regions of hydrous oxide are involved in the oxygen catalysis and dissolution, while only the topmost atomic layers of rutile IrO2 participate in both reactions. Overall our data provide a contribution to the fundamental understanding of the exceptional stability of Ir-oxides towards the oxygen evolution reaction. The proposed approach to a quantitative assessment of the degree of lattice oxygen participation in the oxygen evolution reaction can be further applied to other oxide catalyst systems. © 2019 The Royal Society of Chemistry.
语种英语
scopus关键词Atoms; Catalysts; Degradation; Dissolution; Mass spectrometry; Oxide minerals; Oxygen; Titanium dioxide; Atom probe tomography; Atomic scale structures; Degradation mechanism; Hydrous iridium oxides; Oxygen evolution reaction; Quantitative assessments; Reaction mechanism; Water electrolysis; Iridium compounds; catalysis; catalyst; dissolution; electrokinesis; iridium; isotopic composition; molecular analysis; oxidation; reaction kinetics
来源期刊Energy and Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/162549
作者单位Helmholtz-Zentrum Berlin GmbH, Helmholtz-Institute Erlangen-Nürnberg, Berlin, 14109, Germany; Max-Planck-Institut für Eisenforschung GmbH40237, Germany; Department of Materials Science and Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, 91058, Germany; Institute for Materials and Zentrum fur Grenzflachendominierte Hochstleistungswerkstoffe, Ruhr-Universität Bochum, Bochum, 44780, Germany; Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Erlangen, 91058, Germany; Department of Materials, Royal School of Mines, Imperial College, Prince Consort Road, London, SW7 2BP, United Kingdom; Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, 91058, Germany; Deutsches Zentrum für Luft- und Raumfahrt, Stuttgart, 70569, Germany
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Kasian O.,Geiger S.,Li T.,et al. Degradation of iridium oxides via oxygen evolution from the lattice: Correlating atomic scale structure with reaction mechanisms[J],2019,12(12).
APA Kasian O..,Geiger S..,Li T..,Grote J.-P..,Schweinar K..,...&Mayrhofer K.J.J..(2019).Degradation of iridium oxides via oxygen evolution from the lattice: Correlating atomic scale structure with reaction mechanisms.Energy and Environmental Science,12(12).
MLA Kasian O.,et al."Degradation of iridium oxides via oxygen evolution from the lattice: Correlating atomic scale structure with reaction mechanisms".Energy and Environmental Science 12.12(2019).
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