Two new supramolecular compounds, 2C6H9N2 +. C8H4O4 − .2H2O /(4AMPIP) (1) and C6H9N2 +.C8H5O4 −/(5AMPHIP) (2), were synthesized and characterized by IR spectra, 1H NMR, 13C NMR, and single-crystal X-ray diffraction. Compound 1 crystallizes in the monoclinic system, space group Cc, with a = 7.8914(3), b = 38.4226(16), c = 7.3354(3) Å, β = 107.9460(10)a, V ˚ = 2115.94(15) Å3 , Dc = 1.314 g/cm3 , F(000) = 888, μ =0.10 mm−1 , Z = 4, the final R = 0.0298, and wR = 0.0835 for 3135 observed reflections with I > 2σ(I); and compound 2 crystallizes in the monoclinic system, space group P21/c, with a = 9.0126(2), b = 12.2055(3), c = 12.3170(2) Å, β = 104.2160(10)◦, V = 1313.42(5) Å3 , Dc = 1.387 g/cm3 , F(000) = 576, μ = 0.103 mm−1 , Z = 4, the final R = 0.0454, and wR = 0.1130 for 2799 observed reflections with I > 2σ(I). The 2- amino-4-methylpyridinium (4AMP) and 2-amino-5-methylpyridinium (5AMP) cations are protonated at one of the pyridinium N atoms. In both compounds, the isophthalate anion interacts with protonated cations through a pair of N H···O hydrogen bonds to form a cyclic hydrogen-bonded motif with graph-set notation (R2 2 (8)). In the crystal structure of 1, the ion pairs (whether cation/anion) are linked by water molecules through O H···O, N H···O, and weak C H···O hydrogen bonds, forming a threedimensional network. In the crystal structure of 2, there are chains and layer made up of the O H···O, N H···O, and C H···O hydrogen bonds, forming a two-dimensional network.
