Radiolytic Evaluation of 3,4,3-LI(1,2-HOPO) in Aqueous Solutions

Wang, Yufei; Mezyk, Stephen P.; McLachlan, Jeffrey R.; Grimes, Travis S.; Zalupski, Peter R.; O’Bryan, Hailie T.; Cook, Andrew R.; Abergel, Rebecca J.; Horne, Gregory P.

doi:10.1021/acs.jpcb.3c01469

Radiolytic Evaluation of 3,4,3-LI(1,2-HOPO) in Aqueous Solutions

Journal Article · Fri Apr 21 00:00:00 EDT 2023 · Journal of Physical Chemistry. B

DOI:https://doi.org/10.1021/acs.jpcb.3c01469· OSTI ID:1971486

^[1]; Mezyk, Stephen P. ^[2]; McLachlan, Jeffrey R. ^[3]; ^[4]; ^[4]; O’Bryan, Hailie T. ^[5]; ^[6]; ^[7]; ^[4]

University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)
California State University, Long Beach, CA (United States)
Florida International University (FIU), Miami, FL (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

We report 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 (eaq^-, H^· atom, and ^·OH and NO₃^· radicals). The reaction of HOPO with eaq^- is believed to proceed via reduction of the hydroxypyridinone moiety, while transient adduct spectra indicate that reactions with the H^· atom and ^·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 ([²⁴¹Am^III(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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). Laser Electron Accelerator Facility (LEAF); Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE Office of Nuclear Energy (NE), Nuclear Infrastructure Programs. Nuclear Facility Operations

Grant/Contract Number:: SC0012704; AC07-05ID14517; NE0008659; SC0014664; NE0008949

OSTI ID:: 1971486

Alternate ID(s):: OSTI ID: 1976156

Report Number(s):: BNL-224257-2023-JAAM; INL/JOU-23-71512-Rev000; TRN: US2313576

Journal Information:: Journal of Physical Chemistry. B, Vol. 127, Issue 17; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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