Structural and Thermodynamics Studies on Polyaminophosphonate Ligands for Uranyl Decorporation.

Fiche publication


Date publication

février 2021

Journal

Inorganic chemistry

Auteurs

Membres identifiés du Cancéropôle Est :
Dr CHARBONNIERE Loïc


Tous les auteurs :
Ye G, Roques J, Solari PL, Den Auwer C, Jeanson A, Brandel J, Charbonnière LJ, Wu W, Simoni É

Résumé

The development of actinide decorporation agents with high complexation affinity, high tissue specificity, and low biological toxicity is of vital importance for the sustained and healthy development of nuclear energy. After accidental actinide intake, sequestration by chelation therapy to reduce acute damage is considered as the most effective method. In this work, a series of bis- and tetra-phosphonated pyridine ligands have been designed, synthesized, and characterized for uranyl (UO) decorporation. Owing to the absorption of the ligand and the luminescence of the uranyl ion, UV-vis spectroscopy and time-resolved laser-induced fluorescence spectroscopy (TRLFS) were used to probe complexation and structure variation of the complexes formed by the ligands with uranyl. Density functional theory (DFT) calculations and X-ray absorption fine structure (XAFS) spectroscopy on uranyl-ligand complexes revealed the coordination geometry around the uranyl center at pH 3 and 7.4. High affinity constants (log ∼17) toward the uranyl ion were determined by displacement titration. A preliminary chelation study proves that bis-phosphonated pyridine ligands can remove uranium from calmodulin (CaM) at a low dose and in the short term, which supports further uranyl decorporation applications of these ligands.

Référence

Inorg Chem. 2021 Feb 1;: