Bis(acetonitrile)bis(acetylacetonato)ruthenium(III) mediated chemical transformations of coordinated 2-methylthioanilide

Dalton Transactions : an International Journal of Inorganic Chemistry
Sudipta ChatterjeeSreebrata Goswami

Abstract

Chemical reaction of [Ru(III)(acac)(2)(CH(3)CN)(2)]ClO(4) (1) with 2-methylthioaniline, HL(1) in ethanol under basic conditions yielded three new complexes Ru(II)(acac)(2)(L(1b)) (1b), (L(1b) = 4-imino-3-(methylsulfanyl)cyclohexa-2,5-dien-1-one), Ru(III)(acac)(2)(L(1c)) (1c), (HL(1c) = N-(2-methylthiophenyl)formamide) and (acac)(2)Ru(II)(μ-L(1d))Ru(II)(acac)(2) (1d), (L(1d) = 1,4-bis(2-methylthioaniline)-1,4-diazabutadiene) via the intermediate Ru(III)(acac)(2)(L(1a)) (1a, L(1a) = (L(1))(-) = 2-methylthioanilide). The reaction proceeded through temperature induced valence tautomerisation between the Ru(III) center and its 2-methylthioanilide counterpart in 1a with concomitant reduction of ruthenium from +III to +II oxidation state and oxidation of ligand L(1a), resulting in aromatic ring hydroxylation, N-formylation and C-C bond formation reactions. All the complexes have been characterised by their single-crystal X-ray structure determination and various spectroscopic and electrochemical techniques. The identity of complex 1a has been confirmed by X-ray crystal structure determination of complex 2, a phenyl analogue of complex 1a. The complexes (1a-d) showed intense charge transfer (MLCT/LMCT) transition in the long wavelength...Continue Reading

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