The focus of this thesis is the design of low-dimensional coordination polymers (CPs) using semi-rigid N-donor ligands based on heterocyclic molecules, especially benzotriazole, and the investigation of their potential magnetic and catalytic properties. Chapter 1 serves as a general introduction to the chemistry discussed in the thesis. The first part emphasizes on the synthetic aspects and applications of CPs. The second part presents the unique chemical characteristics of benzotriazole and includes a thorough literature review on its use as a ligand in coordination chemistry, culminating to the development of a ligand system for the design of the targeted materials. Chapter 2 introduces the main family of benzotriazole-based ligands (L1-L3) employed in this thesis, focusing on their coordination chemistry with cobalt salts. The synthesis and characterisation of a series of novel 0D, 1D and 2D compounds with a large structural variety is reported. Synthetic aspects and magnetic properties of selected compounds are discussed. Chapters 3, 4 and 5 report a series of copper coordination compounds employing L1-L3 as well as analogous N-donor ligands (L4-L8). A system of 1D CPs is established and investigated for its catalytic properties in a range of organic transformations that includes the synthesis of 1,4-dihydropyridines through a previously unreported route, the A3 coupling and the ‘click' azide-alkyne cycloaddition reaction. Investigations into optimising the catalytic behaviour and mechanistic aspects of this system are presented. In Chapter 6 the coordination capabilities of L1-L3 are combined with the rich chemistry of silver salts to generate a structurally diverse family of 0D, 1D and 2D compounds. Investigations of their potential catalytic properties in the A3 coupling and alkyne hydration reactions are additionally presented. Chapter 7 provides an overall conclusion to the work presented in the thesis, including its contributions to the reported literature as well as potential future directions. Finally, experimental and synthetic details as well as crystallographic data are presented in Chapter 8 and Chapter 9 respectively.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:759591 |
| Date | January 2018 |
| Creators | Loukopoulos, Edward |
| Publisher | University of Sussex |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | http://sro.sussex.ac.uk/id/eprint/79824/ |
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