Four New Compounds Based on Terephthalate and 2‐(4‐Pyridyl)benzimidazole Ligands

Four new compounds based on H 2 BDC and PyBIm [H 2 BDC = 1,4‐benzenedicarboxylatic acid, PyBIm = 2‐(4‐pyridyl)benzimidazole], (PyBIm)(H 2 BDC) 0.5 ( 1 ), Co(PyBIm) 2 (HBDC)(BDC) 0.5 ( 2 ), Ni(PyBIm) 2 (HBDC)(BDC) 0.5 ( 3 ), and Zn(BDC)(PyBIm) · H 2 O ( 4 ), were synthesized by hydrothermal methods and characterized by X‐ray diffraction. Compound 1 contains two types of hydrogen bonding N–H ··· N and O–H ··· N, which connect the molecules into a two‐dimensional (2D) layer. Complex 2 crystallizes isostructural to 3 in triclinic space group P $\bar{1}$ , in 1D chains. The hydrogen‐bonding interactions between uncoordinated N, N–H and COOH groups in 2 connect the 1D chains into a 2D layer. Complex 4 displays a 1D structure, which is finally extended to a 3D supramolecular framework by hydrogen bonding and π–π packing interactions. The magnetic properties of compounds 2 and 3 were studied as well.