Synthesis and Characterization of a Neutral Titanium Tris(iminosemiquinone) Complex Featuring Redox-Active Ligands
By Clark, Kensha Marie; Bendix, Jesper; Heyduk, Alan F. & Ziller, Joseph W.
Published in Inorganic Chemistry
NULL
2012
Abstract
The neutral tris(semiquinonate) complex [Ti(dmp-BIANisq)3] [dmp-BIANisq = N,N'-bis(3,5-dimethylphenylimino)acenaphthenesemiquinonate] was structurally, spectroscopically, and electrochemically characterized. Solid-state magnetism experiments reveal field-quenchable, enhanced temperature-independent paramagnetism (TIP). Density functional theory calculations employing the experimental geometry predicts a strong antiferromagnetic coupling, leading to an S = 0 ground state, but they also hint at spin frustration and concomitant close-lying, excited states, which cause the observed large TIP by admixture into the ground state. The dmp-BIANisq ligand, which facilitates intramolecular electron transfer, was shown to undergo four quasi-reversible redox processes, demonstrating the ability of the ligand to act as an electron reservoir in complexes of early metals.
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