Abstract

The reaction of ferrocenylene bis(α-nitronyl nitroxide) diradical ( 1; [fc(NIT) 2]) with Co(hfac) 2 produces the reduction of the radical character of 1 with the formation of the diamagnetic ferrocenyl bis(α-imino nitroxide) cation, [fc(IMH) 2H] +, which forms with the [Co(II)hfac 3] −, as the counterion, the complex salt 4. This salt crystallizes in the P 1 ̄ spatial group exhibiting an exotic supramolecular architecture in which the molecular ions are bonded through hydrogen bonds forming single chains with a zipper-like arrangement. Remarkable is the presence in complex salt 4 of two proton tautomeric forms in the [fc(IMH) 2H] + units.

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