SUPRAIMAGINGMACHINES · Ditopic Imaging Agents, Interlocked Sensors and Machines

The development of new innovative approaches for personalised healthcare, and the recognition and sensing of environmentally important pollutants resulting from anthropogenic activities, are extremely important areas in which chemical understanding can contribute enormously to the improved well-being of humanity. In particular, the recognition of anions in aqueous media remains a significant challenge. This project will exploit cation-anion interactions augmented by supramolecular chemistry in the preparation of novel heteroditopic receptor molecules for lanthanide cation- anion ion pair recognition. These have the potential to revolutionise magnetic resonance imaging for personalised healthcare, and will provide interlocked host systems capable of sensing and analyte induced molecular motion. Particular emphasis will be given to the construction of heteroditopic macrocyclic and interlocked host systems designed to recognise lanthanide cation-fluoride anion ion pairs. The stimulus for recognising the fluoride anion stems from its duplicitous nature, where for example high levels in drinking water is causing dental and skeletal fluorosis. In stark contrast, importantly for personalised healthcare, fluoride anion recognition offers the potential development of novel 19F MRI and 18-fluoride PET imaging agents. The programme of work in this proposal centres around three closely integrated and synergistic strands. The common theme is to exploit lanthanide- fluoride ion pair recognition in multimodal imaging (Strand 1), to construct interlocked host structures for fluoride recognition, sensing and molecular machine-like induced switchable behaviour (Strand 2), and to assemble interlocked host systems onto transducing surfaces for analyte induced molecular switching (Strand 3).