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Ru-bis(pyridine)pyrazolate (bpp)-Based Water-Oxidation Catalysts Anchored on TiO2 : The Importance of the Nature and Position of the Anchoring Group
Francàs Forcada, Laia (Institut d'Investigacions Químiques de Catalunya)
Richmond, Craig (Institut d'Investigacions Químiques de Catalunya)
Garrido Barros, Pablo (Institut d'Investigacions Químiques de Catalunya)
Planas, Nora (Institut d'Investigacions Químiques de Catalunya)
Roeser, Stephan (Institut d'Investigacions Químiques de Catalunya)
Benet-Buchholz, Jordi (Universitat Autònoma de Barcelona. Departament de Química)
Escriche Martínez, Lluís (Universitat Autònoma de Barcelona. Departament de Química)
Sala Román, Xavier (Universitat Autònoma de Barcelona. Departament de Química)
Llobet Dalmases, Antoni (Universitat Autònoma de Barcelona. Departament de Química)

Data: 2016
Resum: Three distinct functionalisation strategies have been applied to the in, in-[{RuII(trpy)}2(μ-bpp)(H2O)2]3+ (trpy=2,2':6',2''-terpyridine, bpp=bis(pyridine)pyrazolate) water-oxidation catalyst framework to form new derivatives that can adsorb onto titania substrates. Modifications included the addition of sulfonate, carboxylate, and phosphonate anchoring groups to the terpyridine and bis(pyridyl)pyrazolate ligands. The complexes were characterised in solution by using 1D NMR, 2D NMR, and UV/Vis spectroscopic analysis and electrochemical techniques. The complexes were then anchored on TiO2-coated fluorinated tin oxide (FTO) films, and the reactivity of these new materials as water-oxidation catalysts was tested electrochemically through controlled-potential electrolysis (CPE) with oxygen evolution detected by headspace analysis with a Clark electrode. The results obtained highlight the importance of the catalyst orientation with respect to the titania surface in regard to its capacity to catalytically oxidize water to dioxygen.
Ajuts: Ministerio de Economía y Competitividad CTQ-2013-49075-R
Ministerio de Economía y Competitividad SEV-2013-0319
Ministerio de Economía y Competitividad CTQ2014-52974-REDC
Nota: Altres ajuts: "La Caixa" foundation; COST actions, CM1202 and CM1205
Drets: Tots els drets reservats.
Llengua: Anglès
Document: Article ; recerca ; Versió acceptada per publicar
Matèria: Organic-inorganic hybrid materials ; Redox chemistry ; Ruthenium ; Supported catalysts ; Surfaces and interfaces ; Water splitting ; SDG 7 - Affordable and Clean Energy
Publicat a: Chemistry, Vol. 22, Issue 15 (April 2016) , p. 5261-5268, ISSN 1521-3765

DOI: 10.1002/chem.201504015


Postprint
14 p, 1.3 MB

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