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Equilibrium, kinetic and structural properties of gallium(III) and some divalent metal complexes formed with the new DATAm and DATA5m ligands.

Farkas, Edit and Nagel, Johannes and Waldron, Bradley P. and Parker, David and Tóth, Imre and Brücher, Ernő and Rösch, Frank and Baranyai, Zsolt (2017) 'Equilibrium, kinetic and structural properties of gallium(III) and some divalent metal complexes formed with the new DATAm and DATA5m ligands.', Chemistry : a European journal., 23 (43). pp. 10358-10371.

Abstract

The development of 68Ge/68Ga generators has made the positron-emitting 68Ga isotope widely accessible and raised interest in new chelate complexes of Ga3+. The hexadentate 1,4-di(acetate)-6-methyl[amino(methyl)acetate]perhydro-1,4-diazepane (DATAm) ligand and its bifunctional analogue, 1,4-di(acetate)-6-pentanoic acid[amino(methyl)acetate]perhydro-1,4-diazepane (DATA5m), rapidly form complexes with 68Ga in high radiochemical yield. The stability constants of DATAm and DATA5m complexes formed with Ga3+, Zn2+, Cu2+, Mn2+ and Ca2+ have been determined by using pH potentiometry, spectrophotometry (Cu2+) and 1H and 71Ga NMR spectroscopy (Ga3+). The stability constants of Ga(DATAm) and Ga(DATA5m) complexes are slightly higher than those of Ga(AAZTA). The species distribution calculations indicated the predominance of Ga(L)OH mixed-hydroxo complexes at physiological pH. The 1H and 71Ga NMR spectroscopy studies provided information about the coordinated functional groups of ligands and on the kinetics of exchange between the Ga(L) and Ga(L)OH complexes. The transmetalation reactions between the Ga(L) complexes and Cu2+ citrate (6<pH<8.5) occur through both spontaneous and OH−-assisted dissociation of the Ga(L)OH species. At pH 7.4 and 25 °C, the half-lives of the dissociation of Ga(DATAm), Ga(DATA5m) and Ga(AAZTA) were 11, 44 and 24 h, respectively. Similar half-lives have been obtained for the ligand-exchange reactions between the Ga(L)OH complexes and transferrin. The equilibrium and kinetic data indicate that the Ga(DATA5m) complex is a good 68Ga-based radiodiagnostic candidate.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Status:Peer-reviewed
Publisher Web site:https://doi.org/10.1002/chem.201701508
Publisher statement:This is the accepted version of the following article: Farkas, Edit, Nagel, Johannes, Waldron, Bradley P., Parker, David, Tóth, Imre, Brücher, Ernő, Rösch, Frank & Baranyai, Zsolt (2017). Equilibrium, Kinetic and Structural Properties of Gallium(III) and Some Divalent Metal Complexes Formed with the New DATAm and DATA5m Ligands. Chemistry - A European Journal 23(43): 10358-10371, which has been published in final form athttps://doi.org/10.1002/chem.201701508. This article may be used for non-commercial purposes in accordance With Wiley-VCH Terms and Conditions for self-archiving.
Date accepted:05 April 2017
Date deposited:01 August 2017
Date of first online publication:12 July 2017
Date first made open access:12 July 2018

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