An(III)/Ln(III) solvent extraction: Theoretical and experimental investigation of the role of ligand conformational mobility

Mitrofanov, Artem; Andreadi, Nikolai; Matveev, Petr I.; Zakirova, Gladis G.; Borisova, Nataliya E.; Kalmykov, Stepan N.; Петров, В. Г.

doi:10.1016/j.molliq.2020.115098

Cited by 17 publications

(12 citation statements)

References 63 publications

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“…The preliminary scan of potential energy surface and search of a global energy minimum was performed with a stochastic algorithm described in details in our previous work. [46] All the calculations were done in the orca [47] package.…”

Section: Computational Detailsmentioning

confidence: 99%

Investigating the Bismuth Complexes with Benzoazacrown Tri‐ and Tetra‐Acetates

et al. 2021

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The complexation properties towards Bi 3 + of benzoazacrown ligands with five (H 3 BA3A) and six (H 4 BATA) heteroatoms and corresponding number of acetic arms have been investigated. Complexation constants were determined via potentiometric titration for BA3ABi complex (logβ = 26.2) and refined for BATABi complex (logβ = 31.7). According to NMR, X-ray and EXAFS results, chelation of cation by H 3 BA3A appears to be outside the macrocyclic cavity both in the solid state and in the aqueous solution. This out-cage location despite the high stability constant causes serum and in vivo instability of complex of smaller azacrown H 3 BA3A in contrast to H 4 BATA. Whereas the larger macrocycle and four pendant arms of H 4 BATA provide long-range coordination effectively shielding the cation thereby ensuring high inertness in vitro, low accumulation of the radionuclide in the organs, and fast clearance.

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Section: Computational Detailsmentioning

confidence: 99%

Investigating the Bismuth Complexes with Benzoazacrown Tri‐ and Tetra‐Acetates

et al. 2021

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“…We also applied the DKH , scalar-relativistic functional for the Ac 3+ calculations. The preliminary scan of the potential energy surface and the search of a global energy minimum were performed with a stochastic algorithm described in detail in our previous work . All the calculations were done in the ORCA package .…”

Section: Methodsmentioning

confidence: 99%

Insights into Actinium Complexes with Tetraacetates─AcBATA versus AcDOTA: Thermodynamic, Structural, and Labeling Properties

Matazova,

Egorova,

Zubenko

et al. 2023

Inorg. Chem.

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In the current research, we conducted a comparative study of the Ac 3+ complex with H 4 DOTA and H 4 BATA. The stability constants of the [AcBATA] − and [AcDOTA] − complexes were studied directly by extraction methods. We discovered that the thermodynamic properties of the [AcBATA] − complex are superior to those of [AcDOTA] − . Moreover, the fast kinetics of H 4 BATA complexation with Ac 3+ during the radiolabeling experiment was observed already at room temperature. Ac 3+ was placed inside the macrocyclic cavity of the [AcBATA] − complex, preventing the release of the cation. According to DFT studies, two possible conformations were found, where two pendant arms coordinate with the metal cation on one side of the azacrown cavity and two on the other side, or three pendant arms are located on one side and one on the other. Finally, high inertness in vitro and in vivo of [AcBATA] − was discovered, making the H 4 BATA ligand highly preferable for application as a component of actinium-based radiopharmaceuticals.

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“…The pre-organization energy of the ligands ( i.e. difference between the energies of bonded and free forms of the ligand 35 ) was also calculated. This parameter characterizes the complex-forming ability of the organic molecule.…”

Section: Introductionmentioning

confidence: 99%