The article describes syntheses, crystal structures and magnetic properties of six defective dicubane type Ni II 4 clusters of compositions [Ni II 4 (HL 1 ) 2 (μ 3 -X) 2 (μ 1,1 -N 3 ) 2 (μ 1,3 -carboxylato) 2 ]· nH 2 O (1, X = OMe -, carboxylato = o-benzoylbenzoato, n = 0; 2, X = {(OMe -) 0.83 (N 3 -) 0.17 }, carboxylato = phenyl acetato, n = 2; 3, (6), where H 2 L 1 is 2-Formyl-6-{(2-hydroxy-1,1-dimethyl-ethylimino)-methyl}-4ethyl-phenol, and this is the partially hydrolyzed product of initially employed ligand H 3 L, 2,6-bis-{(2-hydroxy-1,1-dimethyl- [a] Scheme 2. General schematic illustration of synthetic procedure for all the complexes 1-6.Scheme 3. Schematic representation of solvent-dependent and both-way interconversion between 1 and 4. sorption of strong intensity in the range of 1619-1633 cm -1 , which can be assigned to, respectively, aldehyde C=O and imine C=N stretchings. Symmetric and asymmetric stretchings of μ 1,3carboxylato ligands in 1-5 appear as bands of medium inten-Eur. J. Inorg. Chem. 2019, 4625-4636 www.eurjic.org 4627 sity in the ranges, respectively, 1557-1585 cm -1 and 1380-1409 cm -1 . The O-H stretchings of water (in 2, 5 and 6) or of water and hydroxo (in 4) appear as a broad band with the center lying in the range of 3416-3451 cm -1 . 4634 romagnetic in these three compounds (J 1 = -1.16, -7.33 and -5.59 cm -1 , respectively).