Versatile Macrocyclic Platform for the Complexation of [(nat)Y/(90)Y]Yttrium and Lanthanide Ions

Autor: Charlene Harriswangler, Laura Caneda-Martínez, Olivier Rousseaux, David Esteban-Gómez, Olivier Fougère, Rosa Pujales-Paradela, Laura Valencia, M. Isabel Fernández, Nicolas Lepareur, Carlos Platas-Iglesias
Přispěvatelé: Universidade da Coruña, Laboratoire Guerbet / Guerbet Research, Universidade de Vigo, Nutrition, Métabolismes et Cancer (NuMeCan), Université de Rennes (UR)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), C.P.-I., and D.E.-G. thank Ministerio de Ciencia e Innovación (Grant PID2019-108352RJ-I00) and Xunta de Galicia (Grant ED431B 2020/52) for generous financial support. The authors are indebted to Centro de Supercomputación of Galicia (CESGA) for providing the computer facilities. C.H. thanks Ministerio de Ciencia e Innovación (Grant PRE2020-092888) and Xunta de Galicia (Grant ED481A 2021/070) for funding her PhD contracts. N.L. acknowledges Labex IRON (grant no. ANR-11-LABX-0018) and Guerbet for financial support. L.V. is indebted to CACTI (Universidade de Vigo) for X-ray measurements. Funding for open access provided by Universidade da Coruña/CISUG., ANR-11-LABX-0018,IRON,Radiopharmaceutiques Innovants en Oncologie et Neurologie(2011), Laboratoire Guerbet, Jonchère, Laurent, Radiopharmaceutiques Innovants en Oncologie et Neurologie - - IRON2011 - ANR-11-LABX-0018 - LABX - VALID
Jazyk: angličtina
Rok vydání: 2022
Předmět:
Zdroj: Inorganic Chemistry
Inorganic Chemistry, 2022, 61 (16), pp.6209-6222. ⟨10.1021/acs.inorgchem.2c00378⟩
ISSN: 0020-1669
1520-510X
Popis: International audience; We report a macrocyclic ligand (H) based on a 3,6,10,13-tetraaza-1,8(2,6)-dipyridinacyclotetradecaphane platform containing three acetate pendant arms and a benzyl group attached to the fourth nitrogen atom of the macrocycle. The X-ray structures of the Y and Tb complexes reveal nine coordination of the ligand to the metal ions through the six nitrogen atoms of the macrocycle and three oxygen atoms of the carboxylate pendants. A combination of NMR spectroscopic studies (H, C, and Y) and DFT calculations indicated that the structure of the Y complex in the solid state is maintained in an aqueous solution. The detailed study of the emission spectra of the Eu and Tb complexes revealed Ln-centered emission with quantum yields of 7.0 and 60%, respectively. Emission lifetime measurements indicate that the ligand offers good protection of the metal ions from surrounding water molecules, preventing the coordination of water molecules. The Y complex is remarkably inert with respect to complex dissociation, with a lifetime of 1.7 h in 1 M HCl. On the other hand, complex formation is fast (∼1 min at pH 5.4, 2 × 10 M). Studies using the Y-nuclide confirmed fast radiolabeling since [Y]Y is nearly quantitatively formed (radiochemical yield (RCY) > 95) in a short time over a broad range of pH values from ca. 2.4 to 9.0. Challenging experiments in the presence of excess ethylenediaminetetraacetic acid (EDTA) and in human serum revealed good stability of the [Y]Y complex. All of these experiments combined suggest the potential application of H derivatives as Y-based radiopharmaceuticals.
Databáze: OpenAIRE
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