Abstract
The syntheses, crystal structures and magnetic properties are reported of two new and unusual mixed-valence Mn clusters [MnII4MnIVO(mpko)5(MeO-hmp)(mpko-hmp)(H2O)](ClO4)3 (1) and [MnII4MnIVO(ppko)5(MeO-hmp)(ppko-hmp)(H2O)](ClO4)3 (2). They were obtained from the reaction of mpkoH or ppkoH and hmpH with Mn(ClO4)2 in the presence of NaOMe, where mpkoH is methyl(pyridin-2-yl)ketone oxime, ppkoH is phenyl(pyridin-2-yl)ketone oxime, and hmpH is 2-(hydroxymethyl)pyridine. Complex 1 possesses a distorted MnII4 cubane core attached to an external MnIV by the O2− ion. The peripheral ligation includes two unprecedented hemiacetal ligands formed in situ from the reaction of hmpH with MeOH or mpkoH/ppkoH. Solid-state dc and ac magnetic susceptibility measurements established that both 1 and 2 possess an S=7/2 ground state, which was confirmed by ac in-phase susceptibility data. Simulations of the χMT versus T data established the presence of dominant antiferromagnetic exchange interactions, rationalizing the observed ground state.
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