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Material effect in the fuel – coolant interaction : structural characterization of the steam explosion debris and solidification mechanism
No full textCe travail a été réalisé en cotutelle entre l’Université Charles à Prague (République Tchèque) et l'Université de Strasbourg (France). Il a également profité d’une coopération entre l'Institut de Chimie Inorganique de l'Académie des Sciences de République Tchèque et le Commissariat à l'Énergie Atomique et aux Énergies Alternatives (CEA, Cadarache, France). Les résultats des travaux ont contribué au projet OCDE / AEN Serena 2 (Programme portant sur l’étude des effets d'une explosion de vapeur dans un réacteur nucléaire à eau). La thèse présentée se situe dans le domaine de la sûreté nucléaire et de la science des matériaux. Elle traite de l’Interaction Combustible-Réfrigérant (ICR, ou FCI en anglais pour Fuel-Coolant Interaction) susceptible d’intervenir lors d’un accident grave de réacteur nucléaire et actuellement à l’étude dans les programme de R&D. Au cours d’un accident de fusion d’un coeur de réacteur, les matériaux fondus peuvent interagir avec le liquide de refroidissement (eau légère), aussi appelé réfrigérant. Cette interaction peut se produire à l'intérieur de la cuve ou, en cas de rupture de celle-ci, à l'extérieur. Ces deux scénarios sont couramment appelés Interaction Combustible-Réfrigérant en- et hors- cuve et se distinguent de par les conditions du réacteur lors de l’accident : pression du système, degré de sous refroidissement de l’eau, etc. L'interaction entre le combustible fondu et le liquide de refroidissement peut évoluer vers une détonation thermique appelée «explosion de vapeur» qui peut endommager le réacteur, voire compromettre l'intégrité du confinement. Des expériences récentes ont montré que la composition du combustible a un effet majeur sur l’apparition et le rendement d’une telle explosion. En particulier, des comportements différents ont été observés entre un matériau simulant, l'alumine, qui explose très facilement, et diverses compositions de corium prototypique (80 m. % UO2, 20% m.% ZrO2). Cet «effet matériau» a suscité un intérêt nouveau pour les analyses post-expériences des débris issus de l’ICR afin de déterminer les mécanismes qui interviennent au cours de ces phénomènes extrêmement rapides. La thèse est organisée en neuf chapitres. Le chapitre 1 constitue une introduction générale et présente le contexte d’un accident grave d’un réacteur nucléaire. Quelques exemples d’accidents graves (Three Miles Island 1979, Tchernobyl 1986 et Fukushima 2011) sont brièvement abordés. Le chapitre 2 résume les aspects théoriques de l'interaction combustible-réfrigérant. Il est divisé en quatre parties correspondant aux quatre étapes généralement rencontrées lors du mécanisme d’ICR i) Prémélange - le combustible fondu, versé dans l'eau, se fragmente en gouttelettes grossières qui s’isolent d’un film de vapeur. ii) Déclenchement – le film de vapeur entourant les gouttes de combustible est déstabilisé, permettant ainsi la fragmentation fine du combustible. iii) Propagation - la fragmentation du combustible se propage à l’ensemble du prémélange, augmentant ainsi la surface de contact entre le combustible fondu et l’eau. Ceci conduit à une production intense de vapeur à grande échelle. iv) Expansion (explosion) - l'énergie thermique transférée du combustible à l'eau est transformée en travail mécanique de la vapeur.[...]This work has been performed under co-tutelle supervision between Charles University in Prague (Czech Republic) and Strasbourg University (France). It also profited from the background and cooperation of Institute of Inorganic Chemistry Academy of Science of the Czech Republic and French Commission for Atomic and Alternative energies (CEA Cadarache). Results of the work contribute to the OECD/NEA project Serena 2 (Program on Steam Explosion Resolution for Nuclear Applications).Presented thesis can be classed in the scientific field of nuclear safety and material science. It is aimed on the socalled “molten nuclear Fuel – Coolant Interaction” (FCI) that belongs among the recent issues of the nuclear reactorsevere accident R&D. During the nuclear reactor melt down accident the melted reactor load can interact with the coolant (light water). This interaction can be located inside the vessel or outside in the case of vessel break-up. These two scenarios are commonly called in- and ex-vessel FCI and they differ in the conditions such as initial pressure of the system, water sub-cooling etc. The Molten fuel – coolant interaction can progress into thermal detonation called “steam explosion” that can challenge the reactor or containment integrity.Recent experiments have shown that the melt composition has a major effect on the occurrence and yield of such explosion. In particular, different behaviors have been observed between simulant material (alumina), which has important explosion efficiency, and some prototypic corium compositions (80 w. % UO2, 20% w. % ZrO2). This “material effect” has launched a new interest in the post-test analyses of FCI debris in order to estimate the processes occurring during these extremely rapid phenomena. The thesis is organized in nine chapters. The chapter 1 gives the general introduction and context of the nuclear reactor accident. Major nuclear accidents (Three Miles Island 1979, Chernobyl 1986 and Fukushima 2011) are briefly described. The chapter 2 summarizes the theoretical aspects of the fuel – coolant interaction. It is divided in four thematic fields according to the FCI progression. In general, FCI has four stages: i) Premixing – hot melt is poured in water and fragmented in coarse droplets surrounded by steam filmii) Triggering – steam film around melt droplets is destabilized allowing fine fragmentation iii) Propagation – the fine fragmentation propagate through the premixture increasing the melt – water interface area, which leads to large steam production iv) Expansion (explosion) – Thermal energy transferred from the melt to water is changed into mechanical workof the steam.The chapter 3 summarizes the research conducted in different experimental facilities using nonradioactive simulant or radioactive prototypic materials. The chapter 4 shows the results of thermodynamic calculations, by which thepossible chemici reactions between melts and water/steam at high temperatures were modeled. Second part presentsthe results of 1D calculations of radiation heat transfer from FCI materials to water/steam. The chapter 5 describes the material analyses of non-radioactive simulant debris coming from MISTEE experimental research program (KTH, Sweden) and PREMIX, ECO facilities (FZK, Germany). The chapters 6 to 8 describe the material analyses of radioactive prototypic debris coming from KROTOS research program (CEA, France). The KROTOS KS2 test used melt composition 70 w. % UO2 and 30 w. % ZrO2, the KS4 test 80 w. % UO2 and 20 w. % ZrO2, the last KS5 test used suboxidized melt 80.1 w. % UO2 and 11.4 w. % ZrO2 and 8.5 w. % metallic Zr. The chapter 9 concludes the work and presents future perspectives
Effet matériaux lors de l'interaction corium-eau : analyse structurale des débris d'une explosition vapeur et mécanismes de solidification
No full textThis work has been performed under co-tutelle supervision between Charles University in Prague (Czech Republic) and Strasbourg University (France). It also profited from the background and cooperation of Institute of Inorganic Chemistry Academy of Science of the Czech Republic and French Commission for Atomic and Alternative energies (CEA Cadarache). Results of the work contribute to the OECD/NEA project Serena 2 (Program on Steam Explosion Resolution for Nuclear Applications).Presented thesis can be classed in the scientific field of nuclear safety and material science. It is aimed on the socalled “molten nuclear Fuel – Coolant Interaction” (FCI) that belongs among the recent issues of the nuclear reactorsevere accident R&D. During the nuclear reactor melt down accident the melted reactor load can interact with the coolant (light water). This interaction can be located inside the vessel or outside in the case of vessel break-up. These two scenarios are commonly called in- and ex-vessel FCI and they differ in the conditions such as initial pressure of the system, water sub-cooling etc. The Molten fuel – coolant interaction can progress into thermal detonation called “steam explosion” that can challenge the reactor or containment integrity.Recent experiments have shown that the melt composition has a major effect on the occurrence and yield of such explosion. In particular, different behaviors have been observed between simulant material (alumina), which has important explosion efficiency, and some prototypic corium compositions (80 w. % UO2, 20% w. % ZrO2). This “material effect” has launched a new interest in the post-test analyses of FCI debris in order to estimate the processes occurring during these extremely rapid phenomena. The thesis is organized in nine chapters. The chapter 1 gives the general introduction and context of the nuclear reactor accident. Major nuclear accidents (Three Miles Island 1979, Chernobyl 1986 and Fukushima 2011) are briefly described. The chapter 2 summarizes the theoretical aspects of the fuel – coolant interaction. It is divided in four thematic fields according to the FCI progression. In general, FCI has four stages: i) Premixing – hot melt is poured in water and fragmented in coarse droplets surrounded by steam filmii) Triggering – steam film around melt droplets is destabilized allowing fine fragmentation iii) Propagation – the fine fragmentation propagate through the premixture increasing the melt – water interface area, which leads to large steam production iv) Expansion (explosion) – Thermal energy transferred from the melt to water is changed into mechanical workof the steam.The chapter 3 summarizes the research conducted in different experimental facilities using nonradioactive simulant or radioactive prototypic materials. The chapter 4 shows the results of thermodynamic calculations, by which thepossible chemici reactions between melts and water/steam at high temperatures were modeled. Second part presentsthe results of 1D calculations of radiation heat transfer from FCI materials to water/steam. The chapter 5 describes the material analyses of non-radioactive simulant debris coming from MISTEE experimental research program (KTH, Sweden) and PREMIX, ECO facilities (FZK, Germany). The chapters 6 to 8 describe the material analyses of radioactive prototypic debris coming from KROTOS research program (CEA, France). The KROTOS KS2 test used melt composition 70 w. % UO2 and 30 w. % ZrO2, the KS4 test 80 w. % UO2 and 20 w. % ZrO2, the last KS5 test used suboxidized melt 80.1 w. % UO2 and 11.4 w. % ZrO2 and 8.5 w. % metallic Zr. The chapter 9 concludes the work and presents future perspectives.Ce travail a été réalisé en cotutelle entre l’Université Charles à Prague (République Tchèque) et l'Université de Strasbourg (France). Il a également profité d’une coopération entre l'Institut de Chimie Inorganique de l'Académie des Sciences de République Tchèque et le Commissariat à l'Énergie Atomique et aux Énergies Alternatives (CEA, Cadarache, France). Les résultats des travaux ont contribué au projet OCDE / AEN Serena 2 (Programme portant sur l’étude des effets d'une explosion de vapeur dans un réacteur nucléaire à eau). La thèse présentée se situe dans le domaine de la sûreté nucléaire et de la science des matériaux. Elle traite de l’Interaction Combustible-Réfrigérant (ICR, ou FCI en anglais pour Fuel-Coolant Interaction) susceptible d’intervenir lors d’un accident grave de réacteur nucléaire et actuellement à l’étude dans les programme de R&D. Au cours d’un accident de fusion d’un coeur de réacteur, les matériaux fondus peuvent interagir avec le liquide de refroidissement (eau légère), aussi appelé réfrigérant. Cette interaction peut se produire à l'intérieur de la cuve ou, en cas de rupture de celle-ci, à l'extérieur. Ces deux scénarios sont couramment appelés Interaction Combustible-Réfrigérant en- et hors- cuve et se distinguent de par les conditions du réacteur lors de l’accident : pression du système, degré de sous refroidissement de l’eau, etc. L'interaction entre le combustible fondu et le liquide de refroidissement peut évoluer vers une détonation thermique appelée «explosion de vapeur» qui peut endommager le réacteur, voire compromettre l'intégrité du confinement. Des expériences récentes ont montré que la composition du combustible a un effet majeur sur l’apparition et le rendement d’une telle explosion. En particulier, des comportements différents ont été observés entre un matériau simulant, l'alumine, qui explose très facilement, et diverses compositions de corium prototypique (80 m. % UO2, 20% m.% ZrO2). Cet «effet matériau» a suscité un intérêt nouveau pour les analyses post-expériences des débris issus de l’ICR afin de déterminer les mécanismes qui interviennent au cours de ces phénomènes extrêmement rapides. La thèse est organisée en neuf chapitres. Le chapitre 1 constitue une introduction générale et présente le contexte d’un accident grave d’un réacteur nucléaire. Quelques exemples d’accidents graves (Three Miles Island 1979, Tchernobyl 1986 et Fukushima 2011) sont brièvement abordés. Le chapitre 2 résume les aspects théoriques de l'interaction combustible-réfrigérant. Il est divisé en quatre parties correspondant aux quatre étapes généralement rencontrées lors du mécanisme d’ICR i) Prémélange - le combustible fondu, versé dans l'eau, se fragmente en gouttelettes grossières qui s’isolent d’un film de vapeur. ii) Déclenchement – le film de vapeur entourant les gouttes de combustible est déstabilisé, permettant ainsi la fragmentation fine du combustible. iii) Propagation - la fragmentation du combustible se propage à l’ensemble du prémélange, augmentant ainsi la surface de contact entre le combustible fondu et l’eau. Ceci conduit à une production intense de vapeur à grande échelle. iv) Expansion (explosion) - l'énergie thermique transférée du combustible à l'eau est transformée en travail mécanique de la vapeur.[...
Hexafluorosilicic Acid (FSA): from Hazardous Waste to Precious Resource in Obtaining High Value-Added Mesostructured Silica
Full text linkIn this work, industrial waste hexafluorosilicic acid (H2SiF6 or FSA) has been proven to be a low-cost alternative to silicate esters for the synthesis of high-quality MCM-41 (high surface area, high degree of order, narrow pore size distribution, high thermal stability) through a head-to-head comparison between the most common silica precursor, tetraethylorthosilicate (TEOS), and FSA. The effect of different parameters such as temperature, time, hydrothermal treatment, and the presence of ethyl acetate has been explored by studying the textural, structural, and morphological features. On the most promising samples, thermal and hydrothermal stability has been assessed, indicating a higher thermal stability for the FSA-derived sample, due to the thicker walls, and comparable hydrothermal stability. The mother solution treatment has allowed the obtainment of nanostructured fluorite as an additional valuable product and a CTAB-rich ammonia solution for successive synthesis with FSA. Recovery processes for the templating agent entrapped in the MCM-41 mesostructure have also been explored for both FSA- and TEOS-derived samples, showing an easier removal in the case of FSA-MCM-41. Moreover, mesostructured silica derived from FSA has also been proven to be an ideal support to design efficient and regenerable mesostructured iron oxide-based sorbents for H2S removal from syngas, showing similar performance to that of the corresponding nanocomposite prepared from TEOS
An innovative route for uranium carbide synthesis and densification using spark plasma sintering
Full text linkLAUREA MAGISTRALEI carburi misti di uranio e plutonio sono considerati una possibile alternativa agli ossidi misti come combustibile di reattori veloci di quarta generazione (Generation IV). Tuttavia, diversi fattori hanno ostacolato la loro affermazione. Tra questi, uno dei più importanti è rappresentato dalla loro difficile e dispendiosa fabbricazione. Convenzionalmente, polveri di ossido di uranio e grafite vengono usate come precursori per la sintesi dei carburi, sfruttando una reazione chimica detta riduzione carbotermica. Tipicamente, per favorire il contatto fra le due fasi, e quindi migliorare la cinetica della reazione, le polveri di partenza vengono a lungo mescolate. Nonostante ciò, i trattamenti termici successivi, necessari alla produzione dei carburi, richiedono alte temperature e lunghe durate. Questa tesi si pone come obiettivo quello di sviluppare e analizzare un nuovo metodo di sintesi e densificazione di carburi d'uranio, volto a risolvere i problemi sopracitati. In particolare, per migliorare la reattività dei precursori, sono state impiegate soluzioni di nitrato di uranile e acido citrico, come sorgenti, rispettivamente, di ossido di uranio e carbonio. La natura liquida dei precursori, unita all'azione complessante del gruppo citrato nei confronti dello ione uranile, ha consentito di ottenere, dopo una decomposizione termica in argon, un composto (UO2/C) caratterizzato da un’omogenea dispersione delle due fasi. La produzione di carburi di uranio é stata condotta attraverso diverse tipologie di trattamenti termici, che hanno visto l'impiego anche di un dispositivo di Spark Plasma Sintering (SPS), attraverso una configurazione di prova opportunamente adattata allo scopo. L’elevata reattività del composto di partenza e l’efficacia dei suddetti trattamenti hanno consentito di ridurre sensibilmente le temperature e i tempi usualmente richiesti, consentendo anche di ottenere una polvere di carburo estremamente sinterizzabile. Diverse tecniche sperimentali sono state impiegate per ricavare informazioni riguardanti la composizione, la struttura e la morfologia dei campioni prodotti, quali diffrazione a raggi X (XRD), microscopia elettronica a scansione (SEM) e a trasmissione (TEM), tomografia a raggi X.Mixed uranium-plutonium carbides are considered as potential fuels for Generation IV fast reactors. However, high temperature and long periods are required to fabricate them, thus heavily hindering their success as a concrete alternative to mixed oxides fuels. Conventionally, UO2 and C powders, precursors for carbide synthesis, are mechanically blended together through a long milling step to facilitate their interaction. In this thesis, a new synthesis and sintering route for carbides production is proposed. At first, a mixture of nanocrystalline UO2 embedded in amorphous carbon was obtained by thermal decomposition of a solution of uranyl nitrate and citric acid. The liquid nature of the precursors assured an intrinsic homogeneity at a molecular scale, thus enhancing their reactivity, avoiding any milling step. The effects of initial composition, temperature, dwell time, gas/vacuum atmosphere, and thus the overall reaction kinetics were studied performing the carbide synthesis in a conventional furnace or in a modified Spark Plasma Sintering (SPS) facility. The latter turned out to be very suitable for this kind of material, allowing a drastic reduction of the time and temperature usually needed. Furthermore, a fine uranium carbide powder was produced with significantly increased sinterability. In fact, the densification was also performed in SPS reaching high densities in very short times. The occurring phenomena, the phase compositions, the morphology, and the structure of the produced samples have been characterized by different experimental techniques, as (among all) X-ray powder diffraction, scanning and transmission electron microscopy, and X-ray tomography
Going Beyond Counting First Authors in Author Co-citation Analysis
Full text linkThe present study examines one of the fundamental aspects of author co-citation analysis (ACA) - the way co-citation
counts are defined. Co-citation counting provides the data on which all subsequent statistical analyses and mappings
are based, and we compare ACA results based on two different types of co-citation counting - the traditional type that
only counts the first one among a cited work's authors on the one hand and a non-traditional type that takes into
account the first 5 authors of a cited work on the other hand. Results indicate that the picture produced through this non-traditional author co-citation counting contains more coherent author groups and is therefore considerably clearer. However, this picture represents fewer specialties in the research field being studied than that produced through the traditional first-author co-citation counting when the same number of top-ranked authors is selected and analyzed. Reasons for these effects are discussed
Variations on the Author
Full text link“Variations on the Author” discusses two of Eduardo Coutinho’s recent films (Um Dia na Vida, from 2010, and Últimas Conversas, posthumously released in 2015) and their contribution to the general question of documentary authorship. The director’s filmography is characterized by a consistent yet self-effacing form of authorial self-inscription: Coutinho often features as an interviewer that rather than express opinions propels discourses; an interviewer that is good at listening. This mode of self-inscription characterizes him as an author who is not expressive but who is nonetheless markedly present on the screen. In Um Dia na Vida, however, Coutinho is completely absent form the image, while Últimas Conversas, on the contrary, includes a confessional prologue that moves the director from the margins to the center of his films. This article examines the ways in which these works stand out in the filmography of a director who offers new insights into the notion of cinematic authorship
Appropriate Similarity Measures for Author Cocitation Analysis
Full text linkWe provide a number of new insights into the methodological discussion about author cocitation analysis. We first argue that the use of the Pearson correlation for measuring the similarity between authors’ cocitation profiles is not very satisfactory. We then discuss what kind of similarity measures may be used as an alternative to the Pearson correlation. We consider three similarity measures in particular. One is the well-known cosine. The other two similarity measures have not been used before in the bibliometric literature. Finally, we show by means of an example that our findings have a high practical relevance.information science;Pearson correlation;cosine;similarity measure;author cocitation analysis
Dispelling the Myths Behind First-author Citation Counts
Full text linkWe conducted a full-scale evaluative citation analysis study of scholars in the XML research field to explore just how different from each other author rankings resulting from different citation counting methods actually are, and to demonstrate the capability of emerging data and tools on the Web in supporting more realistic citation counting methods. Our results contest some common arguments for the continued
use of first-author citation counts in the evaluation of scholars, such as high correlations between author rankings by first-author citation counts and other citation
counting methods, and high costs of using more realistic citation counting methods that are not well-supported by the ISI databases. It is argued that increasingly available digital full text research papers make it possible for citation analysis studies to go beyond what the ISI databases have directly supported and to employ more
sophisticated methods
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