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Life sciences · Journal article
Inorganic Chemistry · November 6, 2026
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Abstract The development of chelators with diverse coordination properties is essential for expanding the radiometals available for imaging and targeted therapy. We investigate the metal-binding behavior of DO2A-2PA, a trans-picolinic acid-functionalized cyclen chelator, with isotopes of lanthanum (133/155La/natLa), actinium (225Ac), lead (203Pb/212Pb/natPb), and lutetium (117Lu/natLu). Metal complexes were characterized in solution by 1H NMR spectroscopy (natLa3+, natPb2+, and natLu3+) and in the solid state by X-ray crystallography (natLa3+, natPb2+). The solid-state structures revealed a 10-coordinate La3+ complex, whereas Pb2+ engaged only six donor atoms and resided deeper within the cyclen cavity, consistent with shorter M-NDO2A distances in [Pb(H4DO2A-2PA)]2+. Solution-state NMR studies showed fluxional behavior for La3+, Pb2+, and Lu3+ complexes, supported by variable-temperature experiments. Radiolabeling studies demonstrated efficient, quantitative, and ambient-temperature incorporation of [225Ac]Ac3+ and [133/135La]La3+, with the resulting radiocomplexes exhibiting high kinetic inertness in vitro. Although quantitative [203Pb]/[212Pb]Pb2+ labeling was achieved with DO2A-2PA, performance did not exceed DOTAM, and incorporation of [177Lu]Lu3+ remained inefficient even at elevated temperatures. Overall, these results identify DO2A-2PA as a promising chelator for large, hard radiometals particularly [225Ac]Ac3+ and [133/135La]La3+ while underscoring that increased donor-atom density does not universally enhance coordination performance for softer radiometals such as [203Pb]/[212Pb]Pb2+.