NDLI: Thermodynamic stability and relaxation studies of small, triaza-macrocyclic Mn(II) chelates

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Thermodynamic stability and relaxation studies of small, triaza-macrocyclic Mn(II) chelates

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	André, João P. Geraldes, Carlos F. G. C. Bonnet, Célia S. Ferreira, Paula M. T. De Sá, Arsénio Tóth, Éva
Description	Author Affiliation: de Sá A ( Centro de Química, Campus de Gualtar, Universidade do Minho, 4710-057 Braga, Portugal.)
Abstract	Due to its favorable relaxometric properties, $Mn^{2+}$ is an appealing metal ion for magnetic resonance imaging (MRI) contrast agents. This paper reports the synthesis and characterization of three new triazadicarboxylate-type ligands and their $Mn^{2+}$ chelates (NODAHep, 1,4,7-triazacyclononane-1,4-diacetate-7-heptanil; NODABA, 1,4,7-triazacyclononane-1,4-diacetate-7-benzoic acid; and NODAHA, 1,4,7-triazacyclononane-1,4-diacetate-7-hexanoic acid). The protonation constants of the ligands and the stability constants of the chelates formed with $Mn^{2+}$ and the endogenous $Zn^{2+}$ ion have been determined by potentiometry . In overall, the thermodynamic stability of the chelates is lower than that of the corresponding NOTA analogues (NOTA = 1,4,7-triazacyclononane-1,4,7-triacetate), consistent with the decreased number of coordinating carboxylate groups. Variable temperature $^{1}H$ NMRD and $^{17}O$ NMR measurements have been performed on the paramagnetic chelates to provide information on the water exchange rates and the rotational dynamics. The values of the $^{17}O$ chemical shifts are consistent with the presence of one water molecule in the first coordination sphere of $Mn^{2+}.$ The three complexes are in the slow to intermediate regime for the water exchange rate, and they all display relatively high rotational correlation times, which explain the relaxivity values between 4.7 and 5.8 $mM^{−1}$ $s^{−1}$ (20 MHz and 298 K). These relaxivities are higher than expected for $Mn^{2+}$ chelates of such size and comparable to those of small monohydrated $Gd^{3+}$ complexes. The amphiphilic [Mn(NODAHep)] forms micelles above 22 mM (its critical micellar concentration was determined by relaxometry and fluorescence), and interacts with HSA via its alkylic carbon chain providing a 60% relaxivity increase at 20 MHz due to a longer tumbling time.
ISSN	14779226
Issue Number	13
Volume Number	42
e-ISSN	13645447
Journal	Dalton Trans.
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2013-04-07
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Aza Compounds Chemistry Chelating Agents Macrocyclic Compounds Manganese Contrast Media Chemical Synthesis Heterocyclic Compounds Humans Magnetic Resonance Imaging Magnetic Resonance Spectroscopy Micelles Oxygen Isotopes Serum Albumin Metabolism Temperature Thermodynamics Journal Article Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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