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Abstract
The octadentate siderophore analog 3,4,3-LI(1,2-HOPO), denoted 343-HOPO hereafter, is known to have high affinity for both trivalent and tetravalent lanthanide and actinide cations. Here we extend its coordination chemistry to the rare-earth cations Sc3+ and Y3+ and characterize fundamental metal–chelator binding interactions in solution via UV-Vis spectrophotometry, nuclear magnetic resonance spectroscopy, and spectrofluorimetric metal-competition titrations, as well as in the solid-state via single crystal X-ray diffraction. Sc3+ and Y3+ binding with 343-HOPO is found to be robust, with both high thermodynamic stability and fast room temperature radiolabeling, indicating that 343-HOPO is likely a promising chelator for in vivo applications with both metals. As a proof of concept, we prepared a 86Y-343-HOPO complex for in vivo PET imaging, and the results presented herein highlight the potential of 343-HOPO chelated trivalent metal cations for therapeutic and theranostic applications.
Radionuclide pairs 44Sc/47Sc and 86Y/90Y possess great promise in the development of theranostic agents, but realizing the full potential of these isotopes necessitates improving rare-earth chelation chemistry. Here the authors show that a hydroxypyridinone-based ligand is a promising candidate for applications in this arena.
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1 Lawrence Berkeley National Laboratory, Chemical Sciences Division, Berkeley, United States (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551)
2 Lawrence Berkeley National Laboratory, Chemical Sciences Division, Berkeley, United States (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); Physical and Life Sciences, Lawrence Livermore National Laboratory, Glenn T. Seaborg Institute, Livermore, United States (GRID:grid.250008.f) (ISNI:0000 0001 2160 9702)
3 Lawrence Berkeley National Laboratory, Chemical Sciences Division, Berkeley, United States (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); University of California, Department of Chemistry, Berkeley, United States (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878)
4 Lawrence Berkeley National Laboratory, Chemical Sciences Division, Berkeley, United States (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); University of California, Department of Nuclear Engineering, Berkeley, United States (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878)