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Highly Luminescent and Stable Hydroxypyridinonate Complexes: A Step Towards New Curium Decontamination Strategies
Author(s) -
SturzbecherHoehne Manuel,
Kullgren Birgitta,
Jarvis Erin E.,
An Dahlia D.,
Abergel Rebecca J.
Publication year - 2014
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201402103
Subject(s) - chemistry , luminescence , denticity , human decontamination , aqueous solution , metal , chemical stability , ligand (biochemistry) , proton , antenna effect , chelation , in vivo , photochemistry , inorganic chemistry , materials science , organic chemistry , biochemistry , physics , receptor , optoelectronics , quantum mechanics , nuclear physics , microbiology and biotechnology , biology
The photophysical properties, solution thermodynamics, and in vivo complex stabilities of Cm III 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 Cm III , 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 Cm III complexes (log β 110 =21.8(4) for 3,4,3‐LI(1,2‐HOPO) and log β 120 =24.5(5) for 5‐LIO(Me‐3,2‐HOPO)). The in vivo complex stability for both ligands was assessed by using 248 Cm 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 Cm III decontamination agent.