Syntheses, Crystal Structures, and Magnetic Properties of Three Metal‐Nitroxide Complexes with the V‐shaped 4, 4′‐Oxybis(benzoate)

Three new metal–nitroxide complexes {[Ni(NIT4Py) 2 (obb)(H 2 O) 2 ] · 1.5H 2 O} n ( 1 ), {[Co(NIT4Py) 2 (obb)(H 2 O) 2 ] · 2H 2 O} n ( 2 ), and [Co(IM4Py) 2 (obb) 2 (H 2 O) 2 ][Co(IM4Py) 2 (H 2 O) 4 ] · 10H 2 O ( 3 ) with the V‐shaped 4,4′‐oxybis(benzoate) [NIT4Py = 2‐(4′‐pyridyl)‐4,4,5,5‐tetramethylimidazoline‐1‐oxyl‐3‐oxide, IM4Py = 2‐(4′‐pyridyl)‐4,4,5,5‐tetramethylimidazoline‐1‐oxide, and obb = 4, 4′‐oxybis(benzoate) anion] were synthesized and structurally characterized. Single‐crystal X‐ray analyses indicate that complexes 1 and 2 crystallize in neutral one‐dimensional (1D) zigzag chains, in which the nitroxide–metal–nitroxide units are linked by the V‐shaped 4,4′‐oxybis(benzoate) anions, whereas complex 3 consists of isolated mononuclear [Co(IM4Py) 2 (obb) 2 (H 2 O) 2 ] 2– anions and [Co(IM4Py) 2 (H 2 O) 4 ] 2+ ions. Magnetic measurements show that complexes 1 and 2 both exhibit weak antiferromagnetic interactions between the metal ions and the nitroxides.