Radiolytic Evaluation of 3,4,3-LI(1,2-HOPO) in Aqueous Solutions.
J Phys Chem B
; 127(17): 3931-3938, 2023 May 04.
Article
em En
| MEDLINE
| ID: mdl-37084416
ABSTRACT
The octadentate hydroxypyridinone ligand 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO) has been identified as a promising candidate for both chelation and f-element separation technologies, two applications that require optimal performance in radiation environments. However, the radiation robustness of HOPO is currently unknown. Here, we employ a combination of time-resolved (electron pulse) and steady-state (alpha self-radiolysis) irradiation techniques to elucidate the basic chemistry of HOPO and its f-element complexes in aqueous radiation environments. Chemical kinetics were measured for the reaction of HOPO and its Nd(III) ion complex ([NdIII(HOPO)]-) with key aqueous radiation-induced radical transients (eaq-, H⢠atom, and â¢OH and NO3⢠radicals). The reaction of HOPO with the eaq- is believed to proceed via reduction of the hydroxypyridinone moiety, while transient adduct spectra indicate that reactions with the H⢠atom and â¢OH and NO3⢠radicals proceeded by addition to HOPO's hydroxypyridinone rings, potentially allowing for the generation of an extensive suite of addition products. Complementary steady-state 241Am(III)-HOPO complex ([241AmIII(HOPO)]-) irradiations showed the gradual release of 241Am(III) ions with increasing alpha dose up to 100 kGy, although complete ligand destruction was not observed.
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01-internacional
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MEDLINE
Idioma:
En
Ano de publicação:
2023
Tipo de documento:
Article