Two mononuclear seven-coordinate cobalt(II) complexes [Co(L)3(NO3)2] (L = 4-tert-butylpyridine, 1; L = isoquinoline, 2) were prepared and structurally analyzed by single-crystal X-ray crystallography. The coordination spheres of 1 and 2 exhibit distorted pentagonal bipyramid geometry. Analysis of their direct-current magnetic data reveals the existence of easy plane anisotropy (D > 0) with a small transverse anisotropy (E), which was further confirmed by high-field electron paramagnetic resonance (HFEPR) spectroscopy. Field-induced slow magnetic relaxations were observed under the applied dc field in complexes 1 and 2 by alternating-current magnetic susceptibility measurements. Importantly, these complexes are new instances of mononuclear high-coordinate cobalt(II)-based single-molecule magnets.
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