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...

ver descrição completa

Detalhes bibliográficos
Autores: Odrobina, Jann, Scholz, Julius, Pannwitz, Andrea, Francàs, Laia, Dechert, Sesbastian Llobet, Antoni, Jooß, Christian, Meyer, Freanc
Tipo de documento: artigo
Data de publicação:2017
País:España
Recursos:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositório:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/305799
Acesso em linha:http://hdl.handle.net/2072/305799
https://doi.org/10.1021/acscatal.6b02860
Access Level:Acceso aberto
Palavra-chave:electrocatalysis
immobilization
rotating ring disk electrode measurements
ruthenium complexes
water oxidation catalysis
X-ray photoelectron spectroscopy
Descrição
Resumo:<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