Backbone Immobilization of the Bis(bipyridyl)pyrazolate Diruthenium

<p> Efficient catalysts for water oxidation are key to all scenarios for artificial solar water splitting, and, in the case of molecular catalysts, their immobilization on conductive solid supports is considered essential for the construction of a photoelectrochemical cell. In this work, deriv...

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Detalles Bibliográficos
Autores: Odrobina, Jann, Scholz, Julius, Pannwitz, Andrea, Francàs, Laia, Dechert, Sesbastian Llobet, Antoni, Jooß, Christian, Meyer, Freanc
Tipo de recurso: artículo
Fecha de publicación:2017
País:España
Institución: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:2072/305799
Acceso en línea:http://hdl.handle.net/2072/305799
https://doi.org/10.1021/acscatal.6b02860
Access Level:acceso abierto
Palabra clave:electrocatalysis
immobilization
rotating ring disk electrode measurements
ruthenium complexes
water oxidation catalysis
X-ray photoelectron spectroscopy
Descripción
Sumario:<p> Efficient catalysts for water oxidation are key to all scenarios for artificial solar water splitting, and, in the case of molecular catalysts, their immobilization on conductive solid supports is considered essential for the construction of a photoelectrochemical cell. In this work, derivatives of the rugged 3,5-bis(bipyridyl)pyrazolate (bbp)-based diruthenium water oxidation precatalyst [(&mu;-bbp){Ru(py)2}2(&mu;-X)]2+ (X = OAc, CO3H) have been synthesized that are equipped with a carboxylate anchor at the ligand backbone. The para-C6H4COOR (R = Et, H) substituent at the pyrazolate-C4 is shown to not have any significant effect on the electronic properties of the bbp-based diruthenium core, or on the catalytic performance when using CeIV as a chemical oxidant. The bbp-based complex with labile exogenous bicarbonate bridge (4) has been successfully anchored on mesoporous ITO (mesoITO), and the hybrid ITO