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| Content Provider | Royal Society of Chemistry (RSC) |
|---|---|
| Author | Pfeifer, Verena Piccinin, Simone Hävecker, Michael Jones, Travis E. Vélez, Juan J. Velasco Arrigo, Rosa Knop-Gericke, Axel Schlögl, Robert |
| Copyright Year | 2017 |
| Abstract | Water splitting performed in acidic media relies on the exceptional performance of iridium-based materials to catalyze the oxygen evolution reaction (OER). In the present work, we use in situ X-ray photoemission and absorption spectroscopy to resolve the long-standing debate about surface species present in iridium-based catalysts during the OER. We find that the surface of an initially metallic iridium model electrode converts into a mixed-valent, conductive iridium oxide matrix during the OER, which contains OII− and electrophilic OI− species. We observe a positive correlation between the OI− concentration and the evolved oxygen, suggesting that these electrophilic oxygen sites may be involved in catalyzing the OER. We can understand this observation by analogy with photosystem II; their electrophilicity renders the OI− species active in O–O bond formation, i.e. the likely potential- and rate-determining step of the OER. The ability of amorphous iridium oxyhydroxides to easily host such reactive, electrophilic species can explain their superior performance when compared to plain iridium metal or crystalline rutile-type IrO2. |
| Starting Page | 2143 |
| Ending Page | 2149 |
| Page Count | 7 |
| File Format | HTM / HTML PDF |
| ISSN | 20416520 |
| Volume Number | 8 |
| Issue Number | 3 |
| Journal | Chemical Science |
| DOI | 10.1039/c6sc04622c |
| Language | English |
| Publisher | Royal Society of Chemistry |
| Access Restriction | Subscribed |
| Subject Keyword | Spectroscopy Water splitting Oxygen Electrode Chemical bond Photosystem II Photoemission spectroscopy X-ray crystallography Oxygen evolution Extracellular matrix Rate-determining step Iridium Electrophile |
| Content Type | Text |
| Resource Type | Article |
| Subject | Chemistry |
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