Probing activated radioprotection of simple hydrophilic phosphonic acids in aqueous solution

Horne, Gregory P.; Zarzana, Christopher A.; Daubaras, Dayna L.; Pilgrim, Corey D.; Rae, Cathy; Faulkner, Richard F.; Kiddle, James J.; Mezyk, Stephen P.

doi:10.1016/j.radphyschem.2019.108636

Title: Probing activated radioprotection of simple hydrophilic phosphonic acids in aqueous solution

Journal Article · 07 December 2019 · Radiation Physics and Chemistry (1993)

DOI: https://doi.org/10.1016/j.radphyschem.2019.108636 · OSTI ID:1593913

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Idaho National Lab. (INL), Idaho Falls, ID (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States); Idaho State Univ., Pocatello, ID (United States)
California State Univ. (CalState), Long Beach, CA (United States)
Saint Xavier Univ., Chicago, IL (United States)

Prior exploration into the radiation chemistry of the ligand octylphenyl-N,N-diisobutylcarbamoylmethyl phosphine oxide (CMPO) and its analogues demonstrated their ability to undergo activated radioprotection in an organic solvent – a feature most advantageous for spent nuclear fuel reprocessing scenarios. This phenomenon was dependent on these organophosphorus compounds forming a sacrificial complex involving extracted nitric acid and the presence of an adjacent phenylphosphine oxide motif in the molecule. However, the hydrophobic nature of these compounds prevented elucidation of which components were essential for activated radioprotection; for example, does the phenylphosphine oxide motif only require protonation, or simply the presence of complexed nitrate anion(s), or both? To begin to address these questions, we report on the effect of dissolved nitrate on the radiation chemistry of a series of simple hydrophilic phosphonic acids (methyl, ethyl, phenyl, and benzyl) in aqueous solution. An extensive suite of gamma irradiations supported by high performance liquid chromatography and nuclear magnetic resonance techniques was used to demonstrate that all four compounds were unable to undergo activated radioprotection. While some nitrate protection was observed, this was attributed to changes in the available suite of radiolysis products, and not to the formation of nitrate-phosphonic acid sacrificial complexes. The absence of activated radioprotection and evidence for the formation of a [PhPA•NO₃-] complex further supports the necessity of complex formation to activate the radioprotection mechanism.

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Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Nuclear Fuel Cycle and Supply Chain. Office of Advanced Fuels Technologies; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC07-05ID14517; NE0008406; FC02-04ER15533

OSTI ID:: 1593913

Alternate ID(s):: OSTI ID: 1580548; OSTI ID: 1656845

Report Number(s):: INL/JOU-19-56059-Rev000; INL/JOU-19-55983-Rev000; TRN: US2101865

Journal Information:: Radiation Physics and Chemistry (1993), Vol. 170, Issue C; ISSN 0969-806X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Probing activated radioprotection of simple hydrophilic phosphonic acids in aqueous solution

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