Abstract
A tetracyanoethylene (TCNE) bridged coordination polymer, [Mn(cyclen)(μ 2-TCNE)] · TCNE ( 1), (cyclen = 1,4,7,10-tetraazacyclododecane, TCNE = tetracyanoethylene), has been synthesized by combining [Mn II(cyclen)] 2+ and the potassium salt of TCNE radical anion, K[TCNE]. The compound crystallizes in two polymorphs. Both structures feature formal TCNE radical anion ligands in an unusual geminal (or 1,1−) bridging geometry between two high spin Mn(II) centers. The N TCNE–Mn–N TCNE bond angles of two bridging TCNE /− ligands are 88.07(9)° 1a and 85.44(14)° 1b, respectively. Each bridging TCNE /− is π stacked with an uncoordinated TCNE /− to form what can be construed as a diamagnetic dianion, TCNE 2 2 - , containing a 4-center 2-electron (4c/2e −) bond. The results of variable-temperature magnetic susceptibility measurements indicate behavior consistent with weak antiferromagnetic coupling between two Mn(II) centers with no significant contribution of spin from the organic radicals.
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