@article{68bc4de9c24643df8dcd47ca94c3c2d5,
title = "Gamma Radiation-Induced Degradation of Acetohydroxamic Acid (AHA) in Aqueous Nitrate and Nitric Acid Solutions Evaluated by Multiscale Modelling",
abstract = "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 fundamental 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 hydroxylamine (HA) with the oxidizing nitrate radical were measured for the first time using electron pulse radiolysis and used as inputs for the kinetic model. The computer model results are validated by comparison to experimental data from steady-state gamma ray irradiations, for which the agreement is excellent. The presented model accurately predicts the yields of the major degradation products of AHA: acetic acid, HA, nitrous oxide, and molecular hydrogen.",
keywords = "Gamma radiolysis, acetohydroxamic acid, electron pulse radiolysis, multiscale computer modelling, radical-induced kinetics",
author = "Conrad, {Jacy K.} and Mezyk, {Stephen P.} and Isherwood, {Liam H.} and Aliaksandr Baidak and Pilgrim, {Corey D.} and Daniel Whittaker and Orr, {Robin M.} and Pimblott, {Simon M.} and Horne, {Gregory P.}",
note = "Funding Information: This research has been funded by U.S. Department of Energy (DOE) Assistant Secretary for Nuclear Energy, under the Material Recovery and Waste Form Development Campaign, DOE‐Idaho Operations Office Contract DE‐AC07‐05ID14517. The electron pulse irradiation experiments performed at the Brookhaven National Laboratory (BNL) Laser Electron Accelerator Facility (LEAF) of the BNL Accelerator Center for Energy Research were supported by the US‐DOE Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under contract DE‐SC0012704. We acknowledge Cathy Rae and Kastli D. Schaller for establishing the GC and IC analysis methods and for their training on using each instrument. We acknowledge the support of The University of Manchester's Dalton Cumbrian Facility (DCF), a partner in the National Nuclear User Facility, the Engineerind and Physical Sciences Research Council (EPSRC) UK National Ion Beam Centre, and the Henry Royce Institute. The UK authors acknowledge financial support was provided by the Advanced Fuel Cycle Programme as part of the UK Department for Business, Energy and Industrial Strategy's (BEIS) Energy Innovation Programme. Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH.",
year = "2023",
month = mar,
day = "1",
doi = "10.1002/cphc.202200749",
language = "English",
volume = "24",
pages = "e202200749",
journal = "ChemPhysChem",
issn = "1439-4235",
number = "5",
}