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The radionuclide 213 Bi can be applied for targeted α therapy (TAT): a type of nuclear medicine that harnesses α particles to eradicate cancer cells. To use this radionuclide for this application, a bifunctional chelator (BFC) is needed to attach it to a biological targeting vector that can deliver it selectively to cancer cells. Here, we investigated six macrocyclic ligands as potential BFCs, fully characterizing the Bi 3+ complexes by NMR spectroscopy, mass spectrometry, and elemental analysis. Solid-state structures of three complexes revealed distorted coordination geometries about the Bi 3+ center arising from the stereochemically active 6s 2 lone pair. The kinetic properties of the Bi 3+ complexes were assessed by challenging them with a 1000-fold excess of the chelating agent diethylenetriaminepentaacetic acid (DTPA). The most kinetically inert complexes contained the most basic pendent donors. Density functional theory (DFT) and quantum theory of atoms in molecules (QTAIM) calculations were employed to investigate this trend, suggesting that the kinetic inertness is not correlated with the extent of the 6s 2 lone pair stereochemical activity, but with the extent of covalency between pendent donors. Lastly, radiolabeling studies of 213 Bi (30-210 kBq) with three of the most promising ligands showed rapid formation of the radiolabeled complexes at room temperature within 8 min for ligand concentrations as low as 10 -7 M, corresponding to radiochemical yields of &gt;80%, thereby demonstrating the promise of this ligand class for use in 213 Bi TAT.

inorganic chemistry

Tuning the Kinetic Inertness of Bi<sup>3+</sup> Complexes: The Impact of Donor Atoms on Diaza-18-Crown-6 Ligands as Chelators for <sup>213</sup>Bi Targeted Alpha Therapy

Tuning the Kinetic Inertness of Bi3+ Complexes: The Impact of Donor Atoms on Diaza-18-Crown-6 Ligands as Chelators for 213Bi Targeted Alpha Therapy

Tuning the Kinetic Inertness of Bi³⁺ Complexes: The Impact of Donor Atoms on Diaza-18-Crown-6 Ligands as Chelators for ²¹³Bi Targeted Alpha Therapy