Two Ni(II) molecular metallacycles of [Ni(bpz*tz˙)(N)] (1) and [Ni(bpztz˙)(pz(Cl)tz˙)]·1.3CHOH·9.3HO (2) (bpz*tz = 3,6-bis(3,5-dimethyl-pyrazolyl)-1,2,4,5-tetrazine; bpztz = 3,6-bis(3-phenyl-pyrazolyl)-1,2,4,5-tetrazine; and pz(Cl)tz = 3-bis(3-phenyl-pyrazolyl)-6-Cl-1,2,4,5-tetrazine) are reported. The single-crystal X-ray diffraction study reveals that 1 displays a square structure while 2 shows a triangle structure due to the steric effect, both bearing tetrazine radical bridges. Furthermore, magnetic studies reveal that the Ni-radical interaction in 1 is strongly ferromagnetic with a coupling constant () of 90.8 cm in the 2 formalist, while the overall antiferromagnetic behaviour of 2 is presumably due to the compete ferromagnetic (for the Ni-radical interaction with = 95.4 cm) and antiferromagnetic (for the Ni-radical interaction, = -57.5 cm) couplings.
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