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Metal Coordination Properties of a Chromophoric Desferrioxamine (DFO) Derivative: Insight on the Coordination Stoichiometry and Thermodynamic Stability of Zr 4+ Complexes.

Matteo SavastanoFrancesca BoscaroAntonio Bianchi
Published in: Molecules (Basel, Switzerland) (2021)
Desferrioxamine (DFO) is the current "gold standard" chelator for 89 Zr 4+ , which is used to label monoclonal antibodies for applications in immunopositron emission tomography. Recently, controversial data have been reported regarding the speciation and the stability of the complexes formed by DFO with Zr 4+ in solution. To shed some light on this point, we studied the coordination properties in solution ofa chromophoric DFO derivative bearing a substituted pyrimidine residue (DFO - Pm) toward several metal ions (Zr 4+ , Cu 2+ , Zn 2+ , Mg 2+ , Ca 2+ , Na + , K + ). Potentiometric titrations showed that DFO - Pm and pristine DFO form complexes with very similar stoichiometry and stability. DFO - Pm, which can consequently be taken as a model system for DFO, provides a photochemical response to metal coordination that can be used to further define the complexes formed. In the critical case of Zr 4+ , spectrophotometric measurements allowed the verification of the formation of 1:1 and 2:3 complexes that, together with 2:2 complexes form the coordination model that was obtained through the use of our potentiometric measurements. Additionally, mass spectrometry measurements verified the formation of 1:1 and 2:3 complexes and showed that 1:2 species can be easily generated through the fragmentation of the 2:3 species. In conclusion, the results obtained with DFO - Pm validate the complexation model of Zr 4+ /DFO composed of 1:1, 2:2, and 2:3 metal-to-ligand complexes. Convergences and conflicts with other works are addressed.
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