A million Turnover Molecular Anode for Catalytic Water Oxidation
<p> Molecular ruthenium-based water oxidation catalyst precursors of general formula [Ru(tda)(L<sup>i</sup>)<sub>2</sub>] (tda<sup>2−</sup> is [2,2′:6′,2′′-terpyridine]-6,6′′-dicarboxylato...
| Authors: | , , , , , , , , , |
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| Format: | article |
| Publication Date: | 2016 |
| Country: | España |
| Institution: | Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| Repository: | Recercat. Dipósit de la Recerca de Catalunya |
| OAI Identifier: | oai:recercat.cat:2072/305915 |
| Online Access: | http://hdl.handle.net/2072/305915 https://doi.org/10.1002/anie.201609167 |
| Access Level: | Open access |
| Keyword: | electrocatalysis redox properties transition metal complexes water oxidaton catalysis water splitting |
| Summary: | <p> Molecular ruthenium-based water oxidation catalyst precursors of general formula [Ru(tda)(L<sup>i</sup>)<sub>2</sub>] (tda<sup>2−</sup> is [2,2′:6′,2′′-terpyridine]-6,6′′-dicarboxylato; L<sup>1</sup>=4-(pyren-1-yl)-<em>N</em>-(pyridin-4-ylmethyl)butanamide, <strong>1 b</strong>; L<sup>2</sup>=4-(pyren-1-yl)pyridine), <strong>1 c</strong>), have been prepared and thoroughly characterized. Both complexes contain a pyrene group allowing ready and efficiently anchoring via π interactions on multi-walled carbon nanotubes (MWCNT). These hybrid solid state materials are exceptionally stable molecular water-oxidation anodes capable of carrying out more than a million turnover numbers (TNs) at pH 7 with an <em>E</em><sub>app</sub>=1.45 V vs. NHE without any sign of degradation. XAS spectroscopy analysis before, during, and after catalysis together with electrochemical techniques allow their unprecedented oxidative ruggedness to be monitored and verified.</p> |
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