Synthesis And Characterization Of Macrocyclic Rhenium Organometallic Complexes

Author : Jin-Hui Wang
Publisher :
ISBN 13 :
Total Pages : 281 pages
Book Rating : 4.:/5 (18 download)

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Download or read book Rhenium Complexes Based on Triazolyl Derivatives written by Jin-Hui Wang and published by . This book was released on 2017 with total page 281 pages. Available in PDF, EPUB and Kindle. Book excerpt: Rhenium complexes play a significant role in nuclear medicine. Rhenium has been widely used as a surrogate of technetium for a long time, and the promising physical features of 186Re and 188Re, make 186/188Re-complexes promising candidates as therapeutic radiopharmaceuticals.Similarly, the interesting photoactive and photoluminescence properties of non-radioactive Re-complexes make them excellent catalysts, luminescent materials and imaging sensors.Thus, in this work, our goal was to (i) develop, using a click chemistry strategy, multidentate ligands for the stabilization of different rhenium cores [Re(CO)3]+ and [ReO]3+ (M = Re or 188Re) as well as the analogous 99mTc-cores in some examples, (ii) assess the potential of the rhenium(technetium) complexes as imaging (natRe or 99mTc) or therapeutic (188Re) agents. To do so, two rhenium(technetium) specific-chelating systems were used: a semi-rigid tripodal system in the second chapter and a pyta moiety in the third chapter, these two chelators being developed previously in our group. Thus, based on a N2O tridentate click ligand, two different studies were carried out in chapter II. In the first one, two synthetic pathways to a range of potentially N3O tetradentate ligands, designed to coordinate rhenium cores as well as their coordination behaviors towards different rhenium cores (oxidation states +I and +V), were investigated. The first radiolabeling results combined with the recent work reported by Dugave and co-workers indicated that this ligand could be a promising 99mTc-chelator for nuclear imaging applications. As perspectives to this work, the extension of the radiolabelling work using the [188ReVO]3+ core should be performed, and the in vitro stability should be tested under physiological conditions in human plasma and by cysteine exchange experiments. The second study was focused on the development of novel hypoxia-selective 99mTc radiopharmaceuticals. Our semi-rigid tripodal click framework was decorated with an appended nitro group (either a nitrobenzyl group or a metronidazole (Mtz) unit). Different positions were considered and at least only two metronidazole (Mtz)-containing ligands and one nitro group-containing ligand as well as their corresponding tricarbonyl rhenium(I) complexes were obtained and characterized, in particular by electrochemistry. The reduction potentials of NO2 group in complexes [Re(CO)3Cl(L2)] and [Re(CO)3(L6)] were similar to those of reported hypoxic imaging agents, prompting us to further investigate other properties of these complexes. Chapter III was focused on the study of AIE (aggregation-induced emission) effect in tricarbonyl Re(I) complexes, the association of this effect with the intrinsic properties of Re(I) complexes being expected to lead to very attractive compounds. To do that, we combined an organic fluorophore (PBO) which exhibits excellent stability and optical properties, with a tricarbonylrhenium(I) complex based on a pyta unit (either a 2-pyridyl-1,2,3-triazole or a 2-pyridyl-1,2,4-triazole ligands). Four compounds were studied. The X-Ray structures revealed spectacular discrepancies between the two first triazole-based complexes ReL8 and ReL9. Moreover, this study being a novel orientation in our group, this work is a great starting point for further investigations. Various organic dyes and/or structural modifications of the organic moiety will soon be considered in order to develop highly emissive rhenium(I) luminescent probes.