Title

Coordination chemistry of rhenium: Design of radiopharmaceuticals for diagnostics and therapeutics in nuclear medicine

Date of Award

2001

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Chemistry

Advisor(s)

Jon A. Zubieta

Keywords

Rhenium, Radiopharmaceuticals, Diagnostics, Therapeutics, Nuclear medicine

Subject Categories

Chemistry | Life Sciences | Pharmacology | Pharmacology, Toxicology and Environmental Health | Physical Sciences and Mathematics

Abstract

A number of rhenium compounds were synthesized and characterized in an attempt to investigate and expand the coordination chemistry of the widely used medicinal imaging radioisotope technetium-99m. Technetium and rhenium are Group VII cogeners with similar hydrazine and oxo-thiolate chemistries. These periodic similarities have allowed for the study of the non-radioactive metal rhenium instead of the synthetically created technetium, which only exists as radioactive isotopes.

In Chapters 1-4 and 6 we address the "3+1" concept of ligand addition to a Group VII metal-oxo species using tridentate ligands carrying the SSS, SOS, ONS, SN(R)S donor atom set (R = various alkyl or aryl substituted pendant groups) and a monodentate thiol. However. Chapter 5 reveals that in the absence of thiolate donors, the {ReO} 3+ core may expand its coordination sphere to accommodate five additional donor groups, an observation suggesting that "3+2" complexes will provide an alternate strategy for the systematic synthesis of materials exploiting the modification of the tridentate and bidentate ligands.

Chapter 7 explores hydrazines as potential tethers, forming two classes of compounds, namely [MCl 3 (η 1 -NNC 5 H 4 NH)(η 2 -HNNC 5 H 4 N)] and [MCl 3 (η 1 -NNC 4 H 3 N 2 H)(η 2 -HNNC 4 H 3 N 2 )] (M = Re or Mo). The study continued with the exploration of the chlorine substitution with potentially useful thiol and alcohol coligands.

Finally. Chapter 8 uses the "3+1" approach in designing long-chain fatty acids for imaging blood perfusion to the heart muscle (myocardium).

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