A new dinuclear Ru-Hbpp based water oxidation catalyst with a trans-disposition of the Ru-OH
dc.contributor.author
dc.date.accessioned
2015-12-15T10:50:34Z
dc.date.available
2015-12-15T10:50:34Z
dc.date.issued
2011-04-18
dc.identifier.issn
1477-9226
dc.identifier.uri
dc.description.abstract
The bis(2-pyridyl)ethylamine (bpea) ligand has been used as a starting material for the synthesis of dinuclear Ru complexes of general formula trans,fac-{[RunX(bpea)]2(μ-bpp)}m+ (for X = Cl, n = II, m = 1, trans-RuII-Cl, 1+; for X = OH, n = III, m = 3, trans-RuIII-OH, 23+) where the 3,5-bis(2-pyridyl)pyrazolate anionic ligand (bpp) acts as bridging dinucleating ligand, the bpea ligand coordinates in a facial manner and the monodentate ligands X are situated in a trans fashion with regard to one another. These complexes have been characterized in solution by 1D and 2D NMR spectroscopy, UV-vis and electrochemical techniques and in the solid state by X-ray diffraction analysis. The reaction of 1(PF6) with Ag+ generates the corresponding solvated complex where the Cl ligand has been removed as insoluble AgCl, followed by the oxidation of Ru(ii) to Ru(iii) to generate the corresponding dinuclear complex trans-RuIII-OH, 2(PF6)3. The latter has been shown to catalytically oxidize water to molecular dioxygen using Ce(iv) as oxidant. Quantitative gas evolution as a function of time has been monitored on line by both manometry and mass spectroscopy (MS) techniques. Relative initial velocities of oxygen formation together with structural considerations rule out an intramolecular O-O bond formation pathway
dc.description.sponsorship
Support formSOLAR-H2(EU212508) and MICINN(CTQ2010-21497, Consolider Ingenio 2010 CSD2006-0003, CTQ2010-21532-C02-01 and CTQ2009-08328) is gratefully acknowledged
dc.format.mimetype
application/pdf
dc.language.iso
eng
dc.publisher
Royal Society of Chemistry (RSC)
dc.relation
info:eu-repo/grantAgreement/MICINN//CTQ2010-21532-C02-01/ES/MIMETIZACION DE PROCESOS BIOINORGANICOS Y APLICACIONES CATALITICAS CON COMPUESTOS DE METALES DE TRANSICION./
dc.relation.isformatof
Reproducció digital del document publicat a: http://dx.doi.org/10.1039/C0DT00964D
dc.relation.ispartof
© Dalton Transactions, 2011, vol. 40, p. 3640-3646
dc.relation.ispartofseries
Articles publicats (D-Q)
dc.rights
Tots els drets reservats
dc.subject
dc.title
A new dinuclear Ru-Hbpp based water oxidation catalyst with a trans-disposition of the Ru-OH
dc.type
info:eu-repo/semantics/article
dc.rights.accessRights
info:eu-repo/semantics/embargoedAccess
dc.embargo.terms
Cap
dc.date.embargoEndDate
info:eu-repo/date/embargoEnd/2026-01-01
dc.type.version
info:eu-repo/semantics/publishedVersion
dc.identifier.doi
dc.identifier.idgrec
018599
dc.contributor.funder
dc.relation.ProjectAcronym
dc.identifier.eissn
1477-9234