The judicious selection of suitable ligands is vitally important in the construction of novel metal–organic frameworks (MOFs) with fascinating structures and interesting properties. Recently, imidazole‐containing multidentate ligands have received much attention. Two new CdII coordination frameworks, namely, poly[tris{μ‐1,4‐bis[(1H‐imidazol‐1‐yl)methyl]benzene‐κ2N3:N3′}tetrakis(nitrato‐κ2O,O′)dicadmium], [Cd2(NO3)4(C14H14N4)3]n, (I), and poly[[bis{μ3‐1,3,5‐tris[(1H‐imidazol‐1‐yl)methyl]benzene‐κ3N3:N3′:N3′′}cadmium] hexafluorosilicate], {[Cd(C18H18N6)2](SiF6)}n, (II), have been synthesized and characterized by elemental analysis, IR spectroscopy and single‐crystal X‐ray diffraction. In polymer (I), the 1,4‐bis[(1H‐imidazol‐1‐yl)methyl]benzene ligand bridges Cd2+ ions with a distorted seven‐coordinated pentagonal bipyramidal geometry, forming a one‐dimensional ladder chain, and the nitrate anions coordinate to the Cd2+ ions in a terminal bidentate fashion. In the crystal, adjacent chains are further connected by C—H…O hydrogen bonds to generate a two‐dimensional (2D) supramolecular structure. Polymer (II) exhibits a 2D layered structure in which 1,3,5‐tris[(1H‐imidazol‐1‐yl)methyl] benzene ligands join Cd2+ centres having a six‐coordinated octahedral structure. The layers are connected by hexafluorosilicate anions via C—H…F hydrogen‐bond interactions, giving rise to a three‐dimensional supramolecular network structure in the solid state. In addition, powder X‐ray diffraction (PXRD) patterns were recorded, thermogravimetric analyses (TGA) carried out and fluorescence properties investigated.
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