Highly Luminescent and Stable Hydroxypyridinonate Complexes: A Step Towards New Curium Decontamination Strategies |
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| Authors: | Dr. Manuel Sturzbecher‐Hoehne Birgitta Kullgren Erin E. Jarvis Dahlia D. An Dr. Rebecca J. Abergel |
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| Affiliation: | Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (USA) |
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| Abstract: | The photophysical properties, solution thermodynamics, and in vivo complex stabilities of CmIII complexes formed with multidentate hydroxypyridinonate ligands, 3,4,3‐LI(1,2‐HOPO) and 5‐LIO(Me‐3,2‐HOPO), are reported. Both chelators were investigated for their ability to act as antenna chromophores for CmIII, leading to highly sensitized luminescence emission of the metal upon complexation, with long lifetimes (383 and 196 μs for 3,4,3‐LI(1,2‐HOPO) and 5‐LIO(Me‐3,2‐HOPO), respectively) and remarkable quantum yields (45 % and 16 %, respectively) in aqueous solution. The bright emission peaks were used to probe the electronic structure of the 5f complexes and gain insight into ligand field effects; they were also exploited to determine the high (and proton‐independent) stabilities of the corresponding CmIII complexes (log β110=21.8(4) for 3,4,3‐LI(1,2‐HOPO) and log β120=24.5(5) for 5‐LIO(Me‐3,2‐HOPO)). The in vivo complex stability for both ligands was assessed by using 248Cm as a tracer in a rodent model, which provided a direct comparison with the in vitro thermodynamic results and demonstrated the great potential of 3,4,3‐LI(1,2‐HOPO) as a therapeutic CmIII decontamination agent. |
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| Keywords: | actinides curium energy transfer luminescence thermodynamics |
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