This research proposal comprises two projects grouped around the idea of generating new polymeric materials using the technique of subcomponent self-assembly, which allows the preparation of complex structures from simple building blocks that come together around metal-ion templates via coordinative and covalent bond formation. The success of Part A will result in the preparation of double-helical polymers consisting of two self-assembled organic polymer strands that wind around a linear array of copper(I) ions. Initial studies have validated the concepts behind our synthetic strategy, and electrochemical measurements together with DFT calculations indicate a high level of electronic delocalization between the copper ions indicating that these polymers could serve as electrically conductive “molecular wires”. Part B will generate a different series of modular metal-organic polymers, consisting of a poly(imine)chain built up using a high-yielding imine exchange reaction. This chain will be bound to and stabilised by copper(I) ions that are also linked to ancillary ligands that fit snugly around the polymer chain using the idea of “steric complimentarity”. Once we have worked out the scope of the chemical reactions underpinning the formation of these polymers, a wide variety of different polymeric materials are predicted to be accessible. Key properties of these materials, such as strength, flexibility, and conductivity, will be tuneable through the incorporation of different monomer units. The self-assembly reactions used to generate these polymers will be carried out in aqueous solution. Water will be the only by-product of many of the condensation reactions that generate polymers. Our objectives in undertaking this project are twofold: to generate new polymeric materials that might possess useful properties (such as electrical conductivity and the ability to self-repair through dynamic reassembly), and to advance the knowledge of molecular self-assembly.
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