Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes
<p> Electrochemical reduction of the dizaonium complex, [RuII(bda)(NO)(N–N2)2]3+, 23+ (N–N22+ is 4-(pyridin-4-yl) benzenediazonium and bda2– is [2,2′-bipyridine]-6,6′-dicarboxylate), in acetone produces the covalent grafting of this molecular c...
| Autores: | , , , , , , , |
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| Formato: | artículo |
| Fecha de publicación: | 2015 |
| País: | España |
| Recursos: | Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| Repositorio: | Recercat. Dipósit de la Recerca de Catalunya |
| OAI Identifier: | oai:recercat.cat:2072/305797 |
| Acesso em linha: | http://hdl.handle.net/2072/305797 https://doi.org/10.1021/acscatal.5b00132 |
| Access Level: | acceso abierto |
| Palavra-chave: | water oxidation catalysis electrocatalysis water splitting Ru complexes modified graphite electrodes heterogeneous water oxidation catalysis RuO2 |
| Resumo: | <p> Electrochemical reduction of the dizaonium complex, [RuII(bda)(NO)(N–N2)2]3+, 23+ (N–N22+ is 4-(pyridin-4-yl) benzenediazonium and bda2– is [2,2′-bipyridine]-6,6′-dicarboxylate), in acetone produces the covalent grafting of this molecular complex onto glassy carbon (GC) electrodes. Multiple cycling voltammetric experiments on the GC electrode generates hybrid materials labeled as GC-4, with the corresponding Ru-aqua complex anchored on the graphite surface. GC-4 has been characterized at pH = 7.0 by electrochemical techniques and X-ray absorption spectroscopy (XAS) and has been shown to act as an active catalyst for the oxidation of water to dioxygen. This new hybrid material has a lower catalytic performance than its counterpart in homogeneous phase and progressively decomposes to form RuO2 at the electrode surface. Nevertheless the resulting metal oxide attached at the GC electrode surface, GC-RuO2, is a very fast and rugged heterogeneous water oxidation catalyst with TOFis of 300 s–1 and TONs > 45 000. The observed performance is comparable to the best electrocatalysts reported so far, at neutral pH.</p> |
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