Development of a new method for investigating the mechanisms of solid particle dissolution in nitric acid media: Millifluidic study using fluorescent indicators
Identifieur interne : 000C27 ( Main/Exploration ); précédent : 000C26; suivant : 000C28Development of a new method for investigating the mechanisms of solid particle dissolution in nitric acid media: Millifluidic study using fluorescent indicators
Auteurs : Céline Delwaulle [France] ; Alastair Magnaldo [France] ; Andrea Salvatores [France] ; Eric Schaer [France] ; Jean-Léon Houzelot [France] ; Benjamin Rodier [France] ; Emilie Bosse [France]Source :
- Chemical engineering journal : (1996) [ 1385-8947 ] ; 2011.
Descripteurs français
- Pascal (Inist)
- Wicri :
- topic : Déchet radioactif, Combustible, Cartographie.
English descriptors
- KwdEn :
- mix :
Abstract
A key step in existing industrial recycling processes for spent nuclear fuel, after cutting up the spent fuel assemblies, is the continuous dissolution of uranium dioxide in a dissolver containing concentrated nitric acid. The purpose of this study is to enhance our understanding of the phenomena governing the oxide behavior during dissolution, and to acquire new experimental data suitable for modeling and optimizing spent fuel dissolution. The approach adopted involved small scale experiments, which are indispensable for observing, understanding and modeling the phenomena occurring at the solid/liquid interface which control the dissolution reaction. A millifluidic reactor of about 1 mL was developed for the continuous dissolution of millimeter or submillimeter solid particles in a nitric acid stream. New experimental and analytical monitoring techniques were used (observation at the interface by confocal microscopy and epifluorescence, tracking of the species involved, pH monitoring at the interface by fluorometry). Qualification and experimental implementation of these techniques were first conducted on a nonradioactive surrogate, copper. These observations were used to better understand and quantify continuously and in situ the material dissolution mechanisms and the pH variation at the interface, as well as providing data on the behavior of the off-gases. Intermediate species favorable to the reaction were identified, and made it possible to quantify the coupling between hydrodynamics and dissolution kinetics. We were also able to obtain a pH map of the reaction interface, which is very difficult to implement for this type of reaction in corrosive media.
Url:
Affiliations:
- France
- Grand Est, Languedoc-Roussillon, Lorraine (région), Occitanie (région administrative), Île-de-France
- Bagnols sur Cèze, Nancy, Paris La Défense
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administrative)</region><region type="old region" nuts="2">Languedoc-Roussillon</region><settlement type="city">Bagnols sur Cèze</settlement></placeName></affiliation></author><author><name sortKey="Magnaldo, Alastair" sort="Magnaldo, Alastair" uniqKey="Magnaldo A" first="Alastair" last="Magnaldo">Alastair Magnaldo</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Commissariat à l'Énergie Atomique et aux Énergies Alternatives, Marcoule, BP 17171</s1><s2>30207 Bagnols sur Cèze</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Occitanie (région administrative)</region><region type="old region" nuts="2">Languedoc-Roussillon</region><settlement type="city">Bagnols sur Cèze</settlement></placeName></affiliation></author><author><name sortKey="Salvatores, Andrea" sort="Salvatores, Andrea" uniqKey="Salvatores A" first="Andrea" last="Salvatores">Andrea Salvatores</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Commissariat à l'Énergie Atomique et aux Énergies Alternatives, Marcoule, BP 17171</s1><s2>30207 Bagnols sur Cèze</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Occitanie (région administrative)</region><region type="old region" nuts="2">Languedoc-Roussillon</region><settlement type="city">Bagnols sur Cèze</settlement></placeName></affiliation></author><author><name sortKey="Schaer, Eric" sort="Schaer, Eric" uniqKey="Schaer E" first="Eric" last="Schaer">Eric Schaer</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Réactions et Genie des Procédés, ENSIC Nancy, 1 rue Grandville, BP 20451</s1><s2>54001 Nancy</s2><s3>FRA</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName></affiliation></author><author><name sortKey="Houzelot, Jean Leon" sort="Houzelot, Jean Leon" uniqKey="Houzelot J" first="Jean-Léon" last="Houzelot">Jean-Léon Houzelot</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Réactions et Genie des Procédés, ENSIC Nancy, 1 rue Grandville, BP 20451</s1><s2>54001 Nancy</s2><s3>FRA</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName></affiliation></author><author><name sortKey="Rodier, Benjamin" sort="Rodier, Benjamin" uniqKey="Rodier B" first="Benjamin" last="Rodier">Benjamin Rodier</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Réactions et Genie des Procédés, ENSIC Nancy, 1 rue Grandville, BP 20451</s1><s2>54001 Nancy</s2><s3>FRA</s3><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName></affiliation></author><author><name sortKey="Bosse, Emilie" sort="Bosse, Emilie" uniqKey="Bosse E" first="Emilie" last="Bosse">Emilie Bosse</name><affiliation wicri:level="3"><inist:fA14 i1="03"><s1>AREVA NC - TourAREVA. 1 place Jean Millier</s1><s2>92084 Paris La Défense</s2><s3>FRA</s3><sZ>7 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Île-de-France</region><settlement type="city">Paris La Défense</settlement></placeName></affiliation></author></analytic><series><title level="j" type="main">Chemical engineering journal : (1996)</title><title level="j" type="abbreviated">Chem. eng. j. : (1996)</title><idno type="ISSN">1385-8947</idno><imprint><date when="2011">2011</date></imprint></series></biblStruct></sourceDesc><seriesStmt><title level="j" type="main">Chemical engineering journal : (1996)</title><title level="j" type="abbreviated">Chem. eng. j. : (1996)</title><idno type="ISSN">1385-8947</idno></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Bubble</term><term>Cartography</term><term>Confocal microscopy</term><term>Cutting</term><term>Dissolution</term><term>Fuel</term><term>Hydrodynamics</term><term>In situ</term><term>Indicator</term><term>Kinetics</term><term>Liquid solid interface</term><term>Miniaturization</term><term>Modeling</term><term>Optimization</term><term>Qualification</term><term>Radioactive waste</term><term>Reactor</term><term>Recycling</term><term>Solid particle</term><term>Surveillance</term><term>pH</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Particule solide</term><term>Dissolution</term><term>Indicateur</term><term>Recyclage</term><term>Déchet radioactif</term><term>Découpage</term><term>Combustible</term><term>Modélisation</term><term>Optimisation</term><term>Interface liquide solide</term><term>Réacteur</term><term>Surveillance</term><term>Microscopie confocale</term><term>pH</term><term>Qualification</term><term>In situ</term><term>Hydrodynamique</term><term>Cinétique</term><term>Cartographie</term><term>Bulle</term><term>Miniaturisation</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Déchet radioactif</term><term>Combustible</term><term>Cartographie</term></keywords><keywords scheme="mix" xml:lang="en"><term>Dissolution</term><term>Gas bubbles</term><term>In situ monitoring</term><term>Kinetics</term><term>Miniaturization</term><term>Nitric acid</term><term>Reaction interface</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">A key step in existing industrial recycling processes for spent nuclear fuel, after cutting up the spent fuel assemblies, is the continuous dissolution of uranium dioxide in a dissolver containing concentrated nitric acid. The purpose of this study is to enhance our understanding of the phenomena governing the oxide behavior during dissolution, and to acquire new experimental data suitable for modeling and optimizing spent fuel dissolution. The approach adopted involved small scale experiments, which are indispensable for observing, understanding and modeling the phenomena occurring at the solid/liquid interface which control the dissolution reaction. A millifluidic reactor of about 1 mL was developed for the continuous dissolution of millimeter or submillimeter solid particles in a nitric acid stream. New experimental and analytical monitoring techniques were used (observation at the interface by confocal microscopy and epifluorescence, tracking of the species involved, pH monitoring at the interface by fluorometry). Qualification and experimental implementation of these techniques were first conducted on a nonradioactive surrogate, copper. These observations were used to better understand and quantify continuously and in situ the material dissolution mechanisms and the pH variation at the interface, as well as providing data on the behavior of the off-gases. Intermediate species favorable to the reaction were identified, and made it possible to quantify the coupling between hydrodynamics and dissolution kinetics. We were also able to obtain a pH map of the reaction interface, which is very difficult to implement for this type of reaction in corrosive media.</div></front></TEI><affiliations><list><country><li>France</li></country><region><li>Grand Est</li><li>Languedoc-Roussillon</li><li>Lorraine (région)</li><li>Occitanie (région administrative)</li><li>Île-de-France</li></region><settlement><li>Bagnols sur Cèze</li><li>Nancy</li><li>Paris La Défense</li></settlement></list><tree><country name="France"><region name="Occitanie (région administrative)"><name sortKey="Delwaulle, Celine" sort="Delwaulle, Celine" uniqKey="Delwaulle C" first="Céline" last="Delwaulle">Céline Delwaulle</name></region><name sortKey="Bosse, Emilie" sort="Bosse, Emilie" uniqKey="Bosse E" first="Emilie" last="Bosse">Emilie Bosse</name><name sortKey="Houzelot, Jean Leon" sort="Houzelot, Jean Leon" uniqKey="Houzelot J" first="Jean-Léon" last="Houzelot">Jean-Léon Houzelot</name><name sortKey="Magnaldo, Alastair" sort="Magnaldo, Alastair" uniqKey="Magnaldo A" first="Alastair" last="Magnaldo">Alastair Magnaldo</name><name sortKey="Rodier, Benjamin" sort="Rodier, Benjamin" uniqKey="Rodier B" first="Benjamin" last="Rodier">Benjamin Rodier</name><name sortKey="Salvatores, Andrea" sort="Salvatores, Andrea" uniqKey="Salvatores A" first="Andrea" last="Salvatores">Andrea Salvatores</name><name sortKey="Schaer, Eric" sort="Schaer, Eric" uniqKey="Schaer E" first="Eric" last="Schaer">Eric Schaer</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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