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Title: Lanthanide architectures, rotaxanes and responsive d-f assemblies
Author: Tropiano, Manuel
Awarding Body: University of Oxford
Current Institution: University of Oxford
Date of Award: 2013
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This work describes the use of copper catalysed "Click" chemistry in the synthesis of lanthanide containing compounds and outlines the application of the products in modulation of luminescence, anion sensing, bioconjugation and multiemissive probes. Chapter one discusses the fundamental properties of lanthanides with a focus on luminescence and magnetism. A brief literature review on the use of emissive lanthanide probes for sensing application is given. The chapter concludes with an overview on "click" chemistry and its use in the design of lanthanide containing architectures. A redox switchable luminescent lanthanide complex using a ferrocene group as antenna is described in chapter 2. Insights into the mechanism of modulation of the luminescence signal are given. Other complexes containing redox active aryl chromophores were prepared and their luminescence properties elucidated. In chapter three, a lanthanide complex is coupled with a rotaxane by Cu(I) "click" reaction. A detailed study of the anion sensing ability of this supramolecular structure follows. Chapter 4 describes the synthesis of orthogonally functionalised synthons containing azide and alkyne groups that are amenable to form macrocyclic structures upon Cu(I) "click" reaction. Chapter 5 describes the preparation and study of a novel class of lanthanide complexes containing an appended azide group, and their luminescence properties are studied. The chapter continues with the description of heterobimetallic f-f' complexes prepared using Cu(I) "click" chemistry. Chapter six describes the synthesis of lanthanide bioconjugates able to target the dopamine transporter (DAT) protein. Chapter seven delineates the overarching conclusions from the thesis and possible future work in the field, while chapter eight provides experimental procedures.
Supervisor: Faulkner, Stephen ; Beer, Paul Sponsor: Engineering and Physical Sciences Research Council
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: Spectroscopy and molecular structure ; Physical Sciences ; Chemistry & allied sciences ; Inorganic chemistry