Gamma Radiation-Induced Degradation of Acetohydroxamic Acid (AHA) in Aqueous Nitrate and Nitric Acid Solutions Evaluated by Multiscale Modelling

Conrad, Jacy Kathleen; Mezyk, Stephen P.; Isherwood, Liam H.; Baidak, Aliaksandr; Pilgrim, Corey David; Whittaker, Daniel; Orr, Robin M.; Pimblott, Simon M.; Horne, Gregory P.

doi:10.1002/cphc.202200749

Gamma Radiation-Induced Degradation of Acetohydroxamic Acid (AHA) in Aqueous Nitrate and Nitric Acid Solutions Evaluated by Multiscale Modelling

Journal Article · Mon Dec 05 00:00:00 EST 2022 · ChemPhysChem

DOI:https://doi.org/10.1002/cphc.202200749· OSTI ID:1922657

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Idaho National Laboratory (INL), Idaho Falls, ID (United States)
California State University (CalState), Long Beach, CA (United States)
University of Manchester (United Kingdom)
National Nuclear Laboratory Central Laboratory Sellafield, Seascale (United Kingdom)

Acetohydroxamic acid (AHA) has been proposed for inclusion in advanced, single-cycle, used nuclear fuel reprocessing solvent systems for the reduction and complexation of plutonium and neptunium ions. For this application, a detailed description of the degradation of AHA in dilute aqueous nitric acid is required. To this end, we present a comprehensive, multiscale computer model for the coupled radiolytic and hydrolytic degradation of AHA in aqueous sodium nitrate and nitric acid solutions. Rate coefficients for the reactions of AHA and HA with the oxidizing nitrate radical were measured for the first time using pulsed electron radiolysis and used as inputs in the kinetic model. The computer model results are validated by comparison to experimental data from steady state gamma irradiations, for which the agreement is excellent. Here, the presented model accurately predicts the yields of the major degradation products of AHA: acetic acid, hydroxylamine, nitrous oxide, and molecular hydrogen.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: (BEIS) Energy Innovation Programme; USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC07-05ID14517; SC0012704

OSTI ID:: 1922657

Report Number(s):: INL/JOU-22-65915

Journal Information:: ChemPhysChem, Journal Name: ChemPhysChem Journal Issue: - Vol. -; ISSN 1439-4235

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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