Summary: | We studied the synthesis and crystal structures of a new two-dimensional (2D) coordination polymer, {Fe<sup>II</sup>(1-Ethyl-imidazole)<sub>2</sub>[Ni<sup>II</sup>(CN)<sub>4</sub>]}<i><sub>n</sub></i> (<b>1</b>), and one-dimensional (1D) coordination polymers, {Fe<sup>II</sup>(1-benzyl-imidazole)<sub>4</sub>[Ni<sup>II</sup>(CN)<sub>4</sub>]}<i><sub>n</sub></i> (<b>2</b>) and {Fe<sup>II</sup>(1-Allyl-imidazole)<sub>4</sub>[Ni<sup>II</sup>(CN)<sub>4</sub>]}<i><sub>n</sub></i> (<b>3</b>). Compound <b>1</b> has a 2D sheet structure, which is a traditional Hofmann-like structure. In compound <b>1</b>, an octahedral Fe<sup>II</sup> ion is coordinated with the nitrogen atoms of the [Ni<sup>II</sup>(CN)<sub>4</sub>] planar unit at equatorial positions and monodentate imidazole derivatives at axial positions. The layers construct a parallel stacking array. Compounds <b>2</b> and <b>3</b> have a 1D chain structure. In compounds <b>2</b> and <b>3</b>, the Fe<sup>II</sup>N<sub>6</sub> coordination environment is formed with four imidazole ligands and two [Ni<sup>II</sup>(CN)<sub>4</sub>]<sup>2−</sup> metalloligands. In the [Ni<sup>II</sup>(CN)<sub>4</sub>]<sup>2−</sup> unit, two CN substituents act as bidentate ligands that form infinite –Ni–C–N–Fe–N–C–Ni– chains. Herein, we discuss the systematic design of polymeric dimensionality.
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