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Publisher: Royal Society of Chemistry
Languages: English
Types: Article
Subjects: Q1, QD
A series of quadruply bonded dimolybdenum compounds of form Mo2(EE′CC[triple bond, length as m-dash]CPh)4 (EE′ = {NPh}2, Mo2NN; {NPh}O, Mo2NO;{NPh}S, Mo2NS; OO, Mo2OO) have been synthesised by ligand exchange reactions of Mo2(O2CCH3)4 with the acid or alkali metal salt of {PhC[triple bond, length as m-dash]CCEE′}−. The compounds Mo2NO, Mo2NS and Mo2OO were structurally characterised by single crystal X-ray crystallography. The structures show that Mo2NO adopts a cis-2,2 arrangement of the ligands about the Mo24+ core, whereas Mo2NS adopts the trans-2,2 arrangement. The influence of heteroatom substitution on the electronic structure of the compounds was investigated using cyclic voltammetry and UV-Vis spectroscopy. Simple N for O for S substitution in the bridging ligands significantly alters the electronic structure, lowering the energy of the Mo2-δ HOMO and reducing the Mo24+/5+ oxidation potential by up to 0.9 V. A different trend is found in the optoelectronic properties, with the energy of the Mo2-δ-to-ligand-π* transition following the order Mo2OO > Mo2NO > Mo2NN > Mo2NS. Electronic structure calculations employing density functional theory were used to rationalise these observations.
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