We report the selective gelation properties of the copper(II) complexes of N-(4-pyridyl)nicotinamide (4PNA). The morphology of the xerogels was examined by scanning electron microscopy (SEM). The correlation between the X-ray powder diffraction (XRPD) pattern of the xerogels and the single crystal structure of the copper(II) acetate complex suggests that the single crystal X-ray data represent a good structural model for the gel fibers, and that gelation arises from the presence of a 1D hydrogen-bonded chain between gelator amide groups and coordinated anions, while the presence of strongly bound water in non-gelator systems results in the formation of more extensively hydrogen-bonded crystalline networks. The selective gelation of all the copper(II) salts compared to the other metal salts may be attributed to the Jahn–Teller distorted nature of copper(II), which weakens water binding in all copper(II) salts.

The role of metal salts in inducing supramolecular gel network formation was analysed by reacting two pyridyl-N-oxide amides with various diamagnetic zinc(II) and cadmium(II) salts. Metal induced supramolecular gelation was observed for zinc(II) and cadmium(II) chloride complexes in water and the morphologies of the xerogels were analysed by scanning electron microscopy (SEM). The relative gel strength was corroborated with various non-bonding interactions observed in the solid-state structures of zinc(II) complexes using X-ray diffraction. The non-bonding interactions of the pyridyl-N-oxide amides and the metal complexes were compared to find the key interactions responsible for metallogel formation. The anion induced stimuli-responsive property of the metallogels was studied in the presence of halides and cyanide anions. The cadmium(II) gels were stable in presence of two equivalents of halides but the network collapsed in presence of cyanide anion in water and this property can be used to detect cyanide anions in water.

Different co-assembly modes depending on the nature of the solvents observed in multi-component systems with structurally similar components.

We report the crystallisation of three forms of the copper(II) isonicotinate–N-oxide complex and their phase interconversion via solvent-mediated crystal-to-crystal transformation. The different forms of the copper complex have been isolated and characterised by single crystal X-ray diffraction. Gel phase crystallisation performed in hydrogels, low molecular weight gels and gels of a tailored gelator showed crystal habit modification. Crystallisation in aqueous ethanol resulted in the concomitant formation of blue (form-I) and green (form-II/IV) crystals while the use of a low molecular weight gel resulted in the selective crystallization of the blue form-I under identical conditions. Comparison of the gel phase and the solution state crystallisation in various solvent compositions reveals that the blue form-I is the thermodynamically stable form under ambient conditions.