Chemistry of [Ru(tpy)(pap)(L′)n+ (tpy = 2,2′,6′,2″-terpyridine; pap = 2-(phenylazo)pyridine; L′ = Cl−, H2O, CH3CN, 4-picoline, N3−; n = 1,2). X-ray crystal structure of [Ru(tpy)(pap)(CH3CN)](ClO4)2 and catalytic oxidation of water to dioxygen by [Ru(tpy)(pap)(H2O)]2+

Add time:08/20/2019    Source:sciencedirect.com

The reaction of [Ru(tpy)Cl3] with pap has afforded [Ru(tpy)(pap)Cl]+ which has been isolated and characterized as the perchlorate salt. Treatment of [Ru(tpy)(pap)Cl]+ with Ag+ in aqueous solution gives [Ru(tpy)(pap)(H2O)]2+. This aquo-complex has been reacted with three monodentate ligands (L′ = CH3CN, 4-picoline and N3− to afford complexes of type [Ru(tpy)(pap)(L′)]n+. Structure determination of [Ru(tpy)(pap) (CH3CN)](ClO4)2 by X-ray crystallography shows that tpy is coordinated to ruthenium in the usual meridional fashion and the pap ligand is bound to ruthenium with the azo-nitrogen trans to CH3CN. All these complexes except [Ru(tpy)(pap)H2O)]2+ show a Ru(II)–Ru(III) oxidation in the range 1.11–1.50 V vs SCE and three ligand(pap)/(tpy)-based reductions on the negative side of SCE. The aquo-complex shows a RuIIOH2/RuIVO couple in aqueous solution (pH = 1–4), the E° of this oxidation is estimated to be 0.82 V vs SCE. Attempt to chemically oxidize the aquo-complex by Ce4+ in aqueous solution (1 M HClO4) results in the catalytic oxidation of water to dioxygen.

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