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A series of experimental studies is described to explore the properties of stimuli-responsive metallo-supramolecular gels, as well as the nature of the gelation mechanism. Morphological and X-ray diffraction observations suggest gelation occurs via the flocculation of semicrystalline colloidal particles, which results in the gels exhibiting pronounced yielding and thixotropic behavior.

A combination of metal ions in conjunction with bis-ligand monomer metallo-supramolecular polymers to produce supermolecular polyelectrolyte gellike materials, which can exhibit thermo-chemo-, mechanoresponses, as well as light-emitting properties is reported. The nature of the response exhibited by these systems depends on the metal ion and the amount of swelling solvent.

A new synthetic approach to the preparation of intramolecularly collapsed nanoparticles under mild, room temperature conditions has been developed from commercially available vinyl monomers. Reaction of isocyanate functionalized linear copolymers with a diamine in dilute solution leads to the efficient formation of nanoparticles where the diameter of the nanoparticle can be varied by controlling both the molecular weight and mole percentage of isocyanate repeat units. Physical properties for the intramolecularly collapsed nanoparticles were fully consistent with a three-dimensional structure and analysis of the collapse reaction revealed that approximately 75% of the isocyanate groups along the backbone underwent crosslinking with 25% being available for further reaction with mono-functional amines. This stepwise consumption of the isocyanates allows the chemical and physical properties of the nanoparticles to be further tuned and significantly opens up the range of nanoparticles that can be prepared using this mild and highly efficient chemistry.