Year: 2023
Type: article
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 ([Nd III (HOPO)] − ) with key aqueous radiation-induced radical transients (e aq –, H • atom, and • OH and NO 3 • radicals). The reaction of HOPO with the e aq – is believed to proceed via reduction of the hydroxypyridinone moiety, while transient adduct spectra indicate that reactions with the H • atom and • OH and NO 3 • radicals proceeded by addition to HOPO’s hydroxypyridinone rings, potentially allowing for the generation of an extensive suite of addition products. Complementary steady-state 241 Am(III)-HOPO complex ([ 241 Am III (HOPO)] − ) irradiations showed the gradual release of 241 Am(III) ions with increasing alpha dose up to 100 kGy, although complete ligand destruction was not observed.
Language: English
Subfield: Inorganic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
Awards: G1187630603, G1210759672, G127156130, G1847291448, G241279073, G2873784832, G2982867544, G3093756240, G357145406, G3850097093, G4662383146, G473123490, G4755537670, G4972998915, G5455996351, G5633341255, G5765906131, G5857397596, G6733788163, G6965541988, G7463374569, G859423672, NEW AWARD FOR FISCAL YEAR 2017 NUCLEAR ENERGY UNIVERSITY PROGRAMS CONSOLIDATED INNOVATIVE NUCLEAR RESEARCH TO UNIVERSITY OF CALIFORNIA, IRVINE., NUCLEAR ENERGY UNIVERSITY PROGRAMS - NUCLEAR ENERGY UNIVERSITY PROGRAMS CONSOLIDATED INNOVATIVE NUCLEAR RESEARCH - UNIVERSITY OF CALIFORNIA, BERKELEY
OpenAlex ID: W4366605921