Catalytic and topological aspects of Schiff base supported 3d-4f polynuclear coordination complexes

Griffiths, Kieran (2018) Catalytic and topological aspects of Schiff base supported 3d-4f polynuclear coordination complexes. Doctoral thesis (PhD), University of Sussex.

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Abstract

The work presented in this thesis deals with the employment of Schiff base ligands used to synthesise novel 3d-4f polynuclear coordination clusters (PCCs) and the investigation into their potential magnetic, luminescent and catalytic properties.

Chapter one provides a general introduction to the chemistry described in the thesis. It includes a general overview of 3d-4f PCC chemistry and the applications of these materials and previous synthetic strategies for the preparation of Schiff base PCCs. A rationale is presented for the ligands employed in the thesis and a synthetic strategy is devised for the synthesis of specific materials.

The initial chapters are focused on the synthesis of 3d-4f PCCs with novel core topologies and the study of their magnetic properties. Several novel series of 3d-4f PCCs are presented with unique core topologies which are previously unobserved in 3d-4f PCC chemistry. In addition, some of the presented PCCs display single-molecule magnet (SMM) properties or a significant magnetocaloric effect (MCE).

Chapter five bridges synthetic aspects discussed in the previous chapters, with a synthetic study targeting 3d-4f PCCs with a defect dicubane core (2,3M4-1) and introduces the term “isoskeletal” to describe PCCs which possess the same topology or related organic structures with the same host framework but different guests.

Chapters seven to nine are focused on the development of a well characterised isoskeletal family of 3d-4f PCCs with a defect dicubane core and the investigation of their potential catalytic properties in a range of organic reactions including Michael Addition, Friedel-Crafts alkylations and multicomponent reactions. Characterisation of the 3d-4f PCCs is emphasised and verifies the stability of the 2,3M4-1 core in solution. An attempt at understanding the catalytic system and mechanistic aspects is undertaken, which is not explored in previously reported 3d-4f PCC co-operative catalysis.

Chapter ten provides an overall conclusion to the work presented in the thesis, whilst highlighting the contributions of this work to the reported literature.

Item Type: Thesis (Doctoral)
Schools and Departments: School of Life Sciences > Chemistry
Subjects: Q Science > QD Chemistry > QD0450 Physical and theoretical chemistry > QD0474 Complex compounds (including clathrate and coordination compounds, chelates, and hydrates)
Depositing User: Library Cataloguing
Date Deposited: 20 Apr 2018 11:00
Last Modified: 20 Apr 2018 11:00
URI: http://sro.sussex.ac.uk/id/eprint/75278

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