Inorganic–Organic Hybrid Materials: Synthesis and X-Ray Structure of N,N-Dimethylimidazolium Salts [(Me2Im)2] [Cd2(SCN)6] and N,N-Dicyclohexylimidazolium [(Cy2Im)2][Cd2(SCN)6]·C3H6O

Two novel N,Nʹ-dialkylimidazolium thiocyanate–cadmium complexes [(R2Im)2][Cd2(SCN)6] for R=Me (3), and cyclohexyl (4) have been synthesized and characterized by single-crystal X-ray diffraction. Compound 3 crystallizes in the monoclinic unit cell dimensions of 17.468(3), 7.7273(12), 10.6750(16) ?, 104.833(2)°, and space group C2 with two [(Me2Im)2] [Cd2(SCN)6] per unit cell. The two cadmium atoms in 3 are octahedrally coordinated in 4N2S and 2N4S coordination environment, and linking into one-dimensional zigzag chains. Compound 4 belongs to the monoclinic space group Cc with unit cell of dimensions 13.3049(12), 17.5550(16), 20.8012(19) ?, 101.494(2)°, and four [(Cy2Im)2][Cd2(SCN)6]·C3H6O per unit cell. The cadmium atoms in 4 are all 3N3S hexa-coordinated with six bridging SCN- ions in an fac configuration and form infinite zigzag polymeric chains. The infinite chains in 3 form an approximate hexagonal array, making triangular channels which are occupied by N,Nʹ-dimethylimidazolium ions, whereas the chains in 4 form layered structure, and the layers are stacked perpendicularly with respect to the orientation of the infinite anionic chains alternatively. N,Nʹ-dicyclohexylimidazolium cations and solvent molecules fill in between layers.