Versatile Macrocyclic Platform for the Complexation of [ⁿᵃᵗY/⁹⁰Y]Yttrium and Lanthanide Ions
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Versatile Macrocyclic Platform for the Complexation of [ⁿᵃᵗY/⁹⁰Y]Yttrium and Lanthanide IonsAuthor(s)
Date
2022-04-14Citation
Harriswangler, C.; Caneda-Martínez, L.; Rousseaux, O.; Esteban-Gómez, D.; Fougère, O.; Pujales-Paradela, R.; Valencia, L.; Fernández, M. I.; Lepareur, N.; Platas-Iglesias, C. Versatile Macrocyclic Platform for the Complexation of [NatY/90Y]Yttrium and Lanthanide Ions. Inorg. Chem. 2022, 61 (16), 6209–6222. https://doi.org/10.1021/acs.inorgchem.2c00378
Abstract
[Abstract] We report a macrocyclic ligand (H3L6) 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 YL6 and TbL6 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 (1H, 13C, and 89Y) and DFT calculations indicated that the structure of the YL6 complex in the solid state is maintained in an aqueous solution. The detailed study of the emission spectra of the EuL6 and TbL6 complexes revealed Ln3+-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 YL6 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 × 10–5 M). Studies using the 90Y-nuclide confirmed fast radiolabeling since [90Y]YL6 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 [90Y]YL6 complex. All of these experiments combined suggest the potential application of H3L6 derivatives as Y-based radiopharmaceuticals.
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Financiado para publicación en acceso aberto: Universidade da Coruña/CISUG
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Atribución 4.0 Internacional
ISSN
0020-1669
1520-510X
1520-510X