Polytopic diazine ligands and their coordination chemistry

Parsons, Stewart R. (2003) Polytopic diazine ligands and their coordination chemistry. Masters thesis, Memorial University of Newfoundland.

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Abstract

This thesis describes the ligands and related complexes synthesized in an attempt to generate homonuclear high nuclearity metal clusters from a family of related ligands. Self-assembly processes are the intellectual basis of the work and exploration of the magnetic properties of the complexes the ultimate reason for the research. -- Chapter 1 deals with the underlying theoretical and historical principles, it includes a brief introduction to the study of polytopic diazine ligands, and their self-assembly forming clusters. Chapter 1 continues with a discussion of the magnetism of metal clusters, including the different types of magnetic interactions possible and a discussion of molecular magnetism. -- Chapter 2 contains general experimental details and background theory on AC/DC SQUID magnetometry and Mössbauer spectroscopy. It briefly discusses the theory of the general ligand syntheses, and continues to specifically describe the preparation of the individual ligands. -- Chapter 3 discusses the results of the ligand synthesis, beginning with the general properties they all share and then specific ligand properties. Chapter 3 ends with the discussion of, and experimental details of, a number of ligands whose synthesis were unsuccessful but would have been of interest to obtain. -- Chapter 4 deals with the inorganic coordination chemistry of these ligands, identification of the complexes formed and a discussion of their magnetic properties. The magnetic discussion deals with the consequences the structural features of the clusters have on the magnetic properties observed and the structure of the cluster formed. Due to the paucity of X-ray data, the majority of the structural details of the ligands and complexes are inferred mainly from spectral data. -- The Appendices include brief background theory behind the modeling of magnetic exchange behavior in metal clusters (Appendix A), crystal structure data (Appendix B), and χM vs. T data (Appendix C).

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