A series of mononuclear Ni(II) compounds [Ni(pao)2(L)2] (pao- = 2-pyridyloximate, L = pyridine (1), 4-picoline (2), 4-ethylpyridine (3), 4-tert-butylpyridine (4), and N-methylimidazole (5)) were synthesized and characterized. The structures of 1 - 3 were determined by X-ray crystallography and revealed that all compounds have the same structural motif with trans coordination fashion for the identical ligands. For magnetic data, the best-fitting to an S = 1 ground state with the zero-field splitting effect found to have the zero-field splitting parameter |D| of 3 - 4 K in this series. These compounds are good coordination donor building blocks for assembly with Mn(III) salen analogues as coordination acceptor building blocks to form 1-D magnetic chains.
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