Application of a hydroxylamine nitrate stability model to plutonium purification process equipment |
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Institution: | 1. 105903 N. Harrington Rd., West Richland, WA, USA;2. Shaw AREVA MOX Services, LLC, Aiken, SC, USA;1. School of Mechanical, Aerospace and Civil Engineering, University of Manchester, Manchester M13 9PL, UK;2. Moscow Institute of Physics and Technology, Dolgoprudny 141700, Russia;1. CRA-NUT National Council for Agricultural Research, Research Center for Food and Nutrition, Via Ardetina 546, 00178 Rome, Italy;2. Laboratorio di Strutture e Materiali Intelligenti – Università La Sapienza di Roma sede distaccata di Cisterna di Latina, Palazzo Caetani ala nord Via San Pasquale snc., 04012 Cisterna di Latina, LT, Italy;3. INAIL, Via Alessandria 220/e, 00198 Rome, Italy;4. Western Regional Research Center, Agricultural Research Service, United States Department of Agriculture, Albany, CA 94710, USA |
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Abstract: | A mathematical model that predicts hydroxylamine nitrate (HAN) (NH2OH·HNO3) stability is applied to aqueous solutions containing HAN, nitric acid and plutonium that are used in plutonium purification processes. The model estimates the stability of these solutions with respect to the rapid, hazardous, autocatalytic reaction of HAN with nitric acid that generates heat and gas. It also accounts for reaction kinetics, temperature changes, gas generation rates, solution volumes and flow rates, and distribution of plutonium and nitric acid between aqueous and organic phases. The model is applied to three typical process vessels used in solvent extraction purification of plutonium – a countercurrent aqueous/organic plutonium stripping column, an oxidation column used for HAN and hydrazine destruction, and a plutonium rework tank. Both normal and off-normal process scenarios are modeled. Two of the off-normal scenarios lead to the rapid autocatalytic reaction of HAN with nitric acid where heat and gas are generated and that could lead to damage of the process equipment and/or release of hazardous plutonium solution from the vessel. In these two cases, stationary aqueous solutions containing HAN, Pu(III), and nitric acid were allowed to slowly react until conditions for the autocatalytic reaction were reached. |
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Keywords: | Hydroxylamine stability Plutonium Kinetics Nitric acid Model Solvent extraction Process equipment |
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