Two types of 2D [RMI]2[Zn3(BDC)3X2] (Type A) and 3D [Zn(BDC)(H2O)] (Type B) (H2BDC = 1,4-benzenedicarboxylate acid) compounds were synthesized with three kinds of 1-alkyl-3-methyl imidazolium halide ([RMI]X) ionic liquids. Type A is the primary structure model showing a (3,6) network. Type B can be obtained from [BMI]Cl, [AMI]Cl and [AMI]Br media, showing a 4,4-connected {4(2)·8(4)} network. The structure, TG, and fluorescence analyses demonstrate the combination effect of the RMI(+) templating effect and X(-) controlling the structure types. The boundary between Types A and B is from [PMI]Cl, via [BMI]Br, to [AMI]I as the reaction media. The decomposition temperatures of the compounds in Type A decrease with increased RMI(+), while X(-) anions exert the influence that compounds containing Br(-) supply the highest thermal stability. Similarly, with increased RMI(+), or X = I(-), the compounds show red shifts compared to the emissions of the ligand.
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