All the work described in this thesis falls within the domain of supramolecular chemistry. All the themes developed represent significant extensions of those previously developed in the laboratory. The focus has been on polymers, both supramolecular and dynamic covalent (dynamer) types, and their behaviour in solution and at the solid-solution interface.It has been essential to study also various other underlying aspects of this chemistry. Some of the monomers used as a source of new polymers have proven to exhibit unanticipated properties in solution and at interfaces, and a detailed investigation has been devoted to attempting to rationalise their behaviour.The results presented in this thesis provide a deeper understanding of several concepts central to supramolecular and dynamic chemistry. In the first section, it is shown that the multiplication or diversification of the dynamic links within the main chain of a dynamer is an effective strategy for enhancing the sophistication of a polymer system. The second section of the thesis concerns self-assembly processes at solid-solution interfaces and includes a detailed study of one completely unexpected self-assembled entity. The results obtained for this novel species have enabled its detailed characterisation and an analysis of its sensitivity to its environment and chemical stimuli.This work in total advances both an understanding of the nature of complex matter (through embellishment of the variety in dynamic polymers) and of the interactions which lead to its assembly (through the detailed characterisation of new materials).
