Den här uppsatsen hanterar ämnet om ett nukleärt arv och minne genom en fallstudie bunden till fyra identifierade aktörer. Alla fyra arbetar med etablerandet av ett slutförvar för högaktivt och långlivat radioaktivt avfall vilket förväntas vara fortsatt farligt under 100,000-tals år. På grund av det enorma tidsspann det gäller lyfter uppsatsen även koncept så som djup tid och den antropocena tidsåldern som bakgrund till sitt ämnesmaterial. Uppsatsen håller även ett fokus på ansvarsfrågan, då det visade sig att det inte fanns något tydligt svar på frågan om vem som höll det primära ansvaret i frågan av informationsbevaring hos aktörerna, om det ens skulle falla fullkomligen till någon av dem, i deras egna ögon. Uppsatsen är centrerad kring arbetet i Sverige, och inte på en explicit internationell nivå. Genom att använda värdebaserade teorier tillsammans med Pierre Noras teori om platser av minne närmar sig uppsatsen frågan om hur aktörer arbetar med informationsbevaring och kunskapshantering, samt hur minnesinstitutioner så som arkiv kan bidra i deras arbete. Generellt visade det sig att aktörernas arbete med informationsbevaring låg på en primärt teoretisk nivå med lite försök till konkretisering av planer. Olika ideer som är menade att underlätta i processen för långtidsinformationsbevaring presenteras, så som markörer, markeringssystem, och immateriella och materiella minnesplatser. Minnesinstitutioner skulle kunna spela en viktig roll inom informationsbevaring för aktörerna som är ansvariga för slutförvaret, två primära sätt presenteras i uppsatsen, (1) arkivhandlingar, och (2) involverandet av Riksantikvarieämbetet. Detta är en två-årig masteruppsats inom musei- och kulturarvsvetenskap. / This thesis handles the subject of nuclear heritage and memory through a case study surrounding the work with information preservation of 4 identified main actors. The information preservation is in turn centred around the potential establishing of a future final repository for highly active and long-lived radioactive waste, which is expected to still be dangerous within 100,000’s of years. Because of these immense time frames the thesis also takes concepts such as deep time and the Anthropocene into account as background to its subject matter. The thesis holds a focus on the responsibility question, as there turned out to be no unambiguous answer to the question of who were to hold responsibility, if any of them were to hold responsibility, in the eyes of the actors.  The case study is centred around the work in Sweden, and not on an explicitly international scale. By using value-based theories as well as Pierre Nora’s theory of sites of memory the thesis approaches the issue of how actors work with information preservation as well as how memory institutions such as archives can contribute to their efforts.   In general, it is found that the actors’ work with information preservation is primarily theoretical with little attempt at concrete executions of solid plans. Different ideas that are meant to facilitate long-term information preservation are presented, such as markers and marking systems, as well as tangible and intangible sites of memory. Memory institutions could play an important role in information preservation for the actors in charge of the repository, two primary ways this could be the case is presented in this thesis, (1) archival records, and (2) involvement of the Swedish National Heritage Board. This is a two-year master’s thesis in Museum and Cultural Heritage Studies.

Deep geological repository (DGR) for disposal of high-level radioactive waste (HLW) is designed to rely on successive superimposed barrier systems to isolate the waste from the biosphere. This multiple barrier system comprises the natural geological barrier provided by the repository host rock and its surrounding and an engineered barrier system (EBS). The EBS represents the synthetic, engineered materials placed within the natural barrier, comprising array of components such as waste form, waste canisters, buffer materials, backfill and seals. The buffer will enclose the waste canisters from all directions and act as a barrier between canisters and host rock of the repository. It is designed to stabilise the evolving thermo-hydro-mechanical-chemical stresses in the repository over a long period (nearly 1000 years) to retard radionuclides from reaching biosphere. Bentonite clay or bentonite-sand mix have been chosen as buffer materials in EBS design in various countries pursuing deep geological repository method. The bentonite buffer is the most important barrier among the other EBS components for a geological repository. The safety of repository depends to a large extent on proper functioning of buffer over a very long period of time during which it must remain physically, chemically and mineralogically stable. The long term stability of bentonite buffer depends on varying temperature and evolution of groundwater composition of host rocks in a complex way. The groundwater in the vicinity of deep crystalline rock is often characterized by high solute concentrations and the geotechnical engineering response of bentonite buffer could be affected by the dissolved salt concentration of the inflowing ground water. Also during the initial period, radiogenic heat produced in waste canisters would radiate into buffer and the heat generated would lead to drying and some shrinkage of bentonite buffer close to canister. This could alter the dry density, moisture content and in turn the hydro-mechanical properties of bentonite buffer in DGR conditions. India has variety of bentonite deposits in North-Western states of Rajasthan and Gujarat. Previous studies on Indian bentonites suggest that bentonite from Barmer district of Rajasthan (termed as Barmer-1 bentonite) is suitable to serve as buffer material in DGR conditions. Nuclear power agencies of several countries have identified suitable bentonites for use as buffer in DGR through laboratory experiments and large scale underground testing facilities. Physico-chemical, mineralogical and engineering properties of Kunigel VI, Kyungju, GMZ, FoCa clay, MX-80, FEBEX and Avonseal bentonites have been extensively studied by Japan, South Korea, China, Belgium, Sweden, Spain, Canada. It is hence essential to examine the suitability of Barmer-1 bentonite as potential buffer in DGR and compare its physico-chemical and hydromechanical properties with bentonite buffers identified by other countries. The significant factors that impact the long-term stability of bentonite buffer in DGR include variations in moisture content, dry density and pore water chemistry. With a view to address these issues, the hydromechanical response of 70 % Barmer-1 bentonite + 30 % river sand mix (termed bentonite enhanced sand, BES specimens) under varying moisture content, dry density and pore water salt concentration conditions have been examined. The broad scope of the work includes: 1) Characterise the physico-chemical and hydro-mechanical properties of Barmer-1 bentonite from Rajasthan, India and compare its properties with bentonite buffers reported in literature. 2) Examine the influence of variations in dissolved salt concentration (of infiltrating solution), dry density and moisture content of compacted BES specimens on their hydro-mechanical response; the hydro-mechanical properties include, swell pressure, soil water characteristic curve (SWCC), unsaturated hydraulic conductivity, moisture diffusivity and unconfined compression strength. Organization of thesis: After the first introductory chapter, a detailed review of literature is performed to highlight the need for detailed characterisation of physico-chemical and hydromechanical properties of Barmer-1 bentonite for its possible application in DGR in the Indian context. Further, existing literature on hydro-mechanical response of bentonite buffer to changes in physical (degree of saturation/moisture content, dry density) and physico-chemical (solute concentration in pore water) is reviewed to define the scope and objectives of the present thesis in Chapter 2. Chapter 3 presents a detailed experimental programme of the study. Chapter 4 characterises Barmer-1 bentonite for physico-chemical (cation exchange capacity, pore water salinity, exchangeable sodium percentage) and hydro-mechanical properties, such as, swell pressure, saturated permeability, soil water characteristic curve (SWCC) and unconfined compression strength. The properties of Barmer-1 bentonite are compared with bentonite buffers reported in literature and generalized equations for determining swell pressure and saturated permeability coefficient of bentonite buffers are arrived at. Chapter 5 describes a method to determine solute concentrations in the inter-lamellar and free-solutions of compacted BES (bentonite enhanced sand) specimens. The solute concentrations in micro and macro pore solutions are used to examine the role of osmotic flow on swell pressures developed by compacted BES specimens (dry density 1.50-2.00 Mg/m3) inundated with distilled water and NaCl solutions (1000-5000 mg/L). The number of hydration layers developed by the compacted BES specimens on inundation with salt solutions in constant volume swell pressure tests is controlled by cation hydration/osmotic flow. The cation hydration of specimens compacted to dry density of 2.00 Mg/m3 is mainly driven by matric suction prevailing in the clay microtructure as the number of hydration layers developed at wetting equilibrium are independent of the total dissolved solids (TDS) of the wetting solution. Consequently, the swell pressures of specimens compacted to 2.00 Mg/m3 were insensitive to the salt concentration of the inundating solution. The cation hydration of specimens compacted to dry density of 1.50 Mg/m3 is driven by both matric suction (prevailing in the clay micro-structure) and osmotic flow as the number of hydration layers developed at wetting equilibrium is sensitive to the TDS of the wetting solution. Expectedly, the swell pressures of specimens compacted to 1.50 Mg/m3 responded to changes in salt concentration of the inundating solution. The 1.75 Mg/m3 specimens show behaviour that is intermediate to the 1.50 and 2.00 Mg/m3 series specimens. Chapter 6 examines the influence of initial degree of saturation on swell pressures developed by the compacted BES specimens (dry density range: 1.40- 2.00 Mg/m3) on wetting with distilled water from micro-structural considerations. The micro-structure of the bentonite specimens are examined in the compacted and wetted states by performing X-ray diffraction measurements. The initial degree of saturation is varied by adding requisite amount of distilled water to the oven-dried BES mix and compacting the moist mixes to the desired density. The montmorillonite fraction in the BES specimens is responsible for moisture absorption during compaction and development of swell pressure in the constant volume oedometer tests. Consequently, it was considered reasonable to calculate degree of saturation based on EMDD (effective montmorillonite dry density) values and correlate the developed swell pressure values with degree of saturation of montmorillonite voids (Sr,MF). XRD measurements with compacted and wetted specimens demonstrated that if specimens of density series developed similar number of hydration layers on wetting under constant volume condition they exhibited similar swell pressures, as was the case for specimens belonging to 1.40 and 1.50 Mg/m3 series. With specimens belonging to 1.75 and 2.00 Mg/m3 series, greater number of hydration layers were developed by specimens that were less saturated initially (smaller initial Sr,MF) and consequently such specimens developed larger swell pressures. When specimens developed similar number of hydration layers in the wetted state, the compaction dry density determined the swell pressure. Chapter 7 examines the influence of salt concentration of infiltrating solution (sodium chloride concentration ranges from 1000- 5000 mg/L) on SWCC relations, unsaturated permeability and moisture diffusivity of compacted BES specimens. Analysis of the experimental and Brooks and Corey best fit plots revealed that infiltration of sodium chloride solutions had progressively lesser influence on the micro-structure and consequently on the SWCC relations with increase in dry density of the compacted specimens. The micro-structure and SWCC relations of specimens compacted to 1.50 Mg/m3 were most affected, specimens compacted to 1.75 Mg/m3 were less affected, while specimens compacted to 2.00 Mg/m3 were unaffected by infiltration of sodium chloride solutions. Variations in dry density of compacted bentonite impacts the pore space available for moisture flow, while, salinity of wetting fluid impacts the pore structure from associated physico-chemical changes in clay structure. Experimental results showed that the unsaturated permeability coefficient is insensitive to variations in dry density and solute concentration of wetting liquid, while, the effective hydraulic diffusivity is impacted by variations in these parameters. Chapter 8 summarises the major findings of the study.

Deep geological repository (DGR) for disposal of high-level radioactive waste (HLW) is designed to rely on successive superimposed barrier systems to isolate the waste from the biosphere. This multiple barrier system comprises the natural geological barrier provided by the repository host rock and its surrounding and an engineered barrier system (EBS). The EBS represents the synthetic, engineered materials placed within the natural barrier, comprising array of components such as waste form, waste canisters, buffer materials, backfill and seals. The buffer will enclose the waste canisters from all directions and act as a barrier between canisters and host rock of the repository. It is designed to stabilise the evolving thermo-hydro-mechanical-chemical stresses in the repository over a long period (nearly 1000 years) to retard radionuclides from reaching biosphere. Bentonite clay or bentonite-sand mix have been chosen as buffer materials in EBS design in various countries pursuing deep geological repository method. The bentonite buffer is the most important barrier among the other EBS components for a geological repository. The safety of repository depends to a large extent on proper functioning of buffer over a very long period of time during which it must remain physically, chemically and mineralogically stable. The long term stability of bentonite buffer depends on varying temperature and evolution of groundwater composition of host rocks in a complex way. The groundwater in the vicinity of deep crystalline rock is often characterized by high solute concentrations and the geotechnical engineering response of bentonite buffer could be affected by the dissolved salt concentration of the inflowing ground water. Also during the initial period, radiogenic heat produced in waste canisters would radiate into buffer and the heat generated would lead to drying and some shrinkage of bentonite buffer close to canister. This could alter the dry density, moisture content and in turn the hydro-mechanical properties of bentonite buffer in DGR conditions. India has variety of bentonite deposits in North-Western states of Rajasthan and Gujarat. Previous studies on Indian bentonites suggest that bentonite from Barmer district of Rajasthan (termed as Barmer-1 bentonite) is suitable to serve as buffer material in DGR conditions. Nuclear power agencies of several countries have identified suitable bentonites for use as buffer in DGR through laboratory experiments and large scale underground testing facilities. Physico-chemical, mineralogical and engineering properties of Kunigel VI, Kyungju, GMZ, FoCa clay, MX-80, FEBEX and Avonseal bentonites have been extensively studied by Japan, South Korea, China, Belgium, Sweden, Spain, Canada. It is hence essential to examine the suitability of Barmer-1 bentonite as potential buffer in DGR and compare its physico-chemical and hydromechanical properties with bentonite buffers identified by other countries. The significant factors that impact the long-term stability of bentonite buffer in DGR include variations in moisture content, dry density and pore water chemistry. With a view to address these issues, the hydromechanical response of 70 % Barmer-1 bentonite + 30 % river sand mix (termed bentonite enhanced sand, BES specimens) under varying moisture content, dry density and pore water salt concentration conditions have been examined. The broad scope of the work includes: 1) Characterise the physico-chemical and hydro-mechanical properties of Barmer-1 bentonite from Rajasthan, India and compare its properties with bentonite buffers reported in literature. 2) Examine the influence of variations in dissolved salt concentration (of infiltrating solution), dry density and moisture content of compacted BES specimens on their hydro-mechanical response; the hydro-mechanical properties include, swell pressure, soil water characteristic curve (SWCC), unsaturated hydraulic conductivity, moisture diffusivity and unconfined compression strength. Organization of thesis: After the first introductory chapter, a detailed review of literature is performed to highlight the need for detailed characterisation of physico-chemical and hydromechanical properties of Barmer-1 bentonite for its possible application in DGR in the Indian context. Further, existing literature on hydro-mechanical response of bentonite buffer to changes in physical (degree of saturation/moisture content, dry density) and physico-chemical (solute concentration in pore water) is reviewed to define the scope and objectives of the present thesis in Chapter 2. Chapter 3 presents a detailed experimental programme of the study. Chapter 4 characterises Barmer-1 bentonite for physico-chemical (cation exchange capacity, pore water salinity, exchangeable sodium percentage) and hydro-mechanical properties, such as, swell pressure, saturated permeability, soil water characteristic curve (SWCC) and unconfined compression strength. The properties of Barmer-1 bentonite are compared with bentonite buffers reported in literature and generalized equations for determining swell pressure and saturated permeability coefficient of bentonite buffers are arrived at. Chapter 5 describes a method to determine solute concentrations in the inter-lamellar and free-solutions of compacted BES (bentonite enhanced sand) specimens. The solute concentrations in micro and macro pore solutions are used to examine the role of osmotic flow on swell pressures developed by compacted BES specimens (dry density 1.50-2.00 Mg/m3) inundated with distilled water and NaCl solutions (1000-5000 mg/L). The number of hydration layers developed by the compacted BES specimens on inundation with salt solutions in constant volume swell pressure tests is controlled by cation hydration/osmotic flow. The cation hydration of specimens compacted to dry density of 2.00 Mg/m3 is mainly driven by matric suction prevailing in the clay microtructure as the number of hydration layers developed at wetting equilibrium are independent of the total dissolved solids (TDS) of the wetting solution. Consequently, the swell pressures of specimens compacted to 2.00 Mg/m3 were insensitive to the salt concentration of the inundating solution. The cation hydration of specimens compacted to dry density of 1.50 Mg/m3 is driven by both matric suction (prevailing in the clay micro-structure) and osmotic flow as the number of hydration layers developed at wetting equilibrium is sensitive to the TDS of the wetting solution. Expectedly, the swell pressures of specimens compacted to 1.50 Mg/m3 responded to changes in salt concentration of the inundating solution. The 1.75 Mg/m3 specimens show behaviour that is intermediate to the 1.50 and 2.00 Mg/m3 series specimens. Chapter 6 examines the influence of initial degree of saturation on swell pressures developed by the compacted BES specimens (dry density range: 1.40- 2.00 Mg/m3) on wetting with distilled water from micro-structural considerations. The micro-structure of the bentonite specimens are examined in the compacted and wetted states by performing X-ray diffraction measurements. The initial degree of saturation is varied by adding requisite amount of distilled water to the oven-dried BES mix and compacting the moist mixes to the desired density. The montmorillonite fraction in the BES specimens is responsible for moisture absorption during compaction and development of swell pressure in the constant volume oedometer tests. Consequently, it was considered reasonable to calculate degree of saturation based on EMDD (effective montmorillonite dry density) values and correlate the developed swell pressure values with degree of saturation of montmorillonite voids (Sr,MF). XRD measurements with compacted and wetted specimens demonstrated that if specimens of density series developed similar number of hydration layers on wetting under constant volume condition they exhibited similar swell pressures, as was the case for specimens belonging to 1.40 and 1.50 Mg/m3 series. With specimens belonging to 1.75 and 2.00 Mg/m3 series, greater number of hydration layers were developed by specimens that were less saturated initially (smaller initial Sr,MF) and consequently such specimens developed larger swell pressures. When specimens developed similar number of hydration layers in the wetted state, the compaction dry density determined the swell pressure. Chapter 7 examines the influence of salt concentration of infiltrating solution (sodium chloride concentration ranges from 1000- 5000 mg/L) on SWCC relations, unsaturated permeability and moisture diffusivity of compacted BES specimens. Analysis of the experimental and Brooks and Corey best fit plots revealed that infiltration of sodium chloride solutions had progressively lesser influence on the micro-structure and consequently on the SWCC relations with increase in dry density of the compacted specimens. The micro-structure and SWCC relations of specimens compacted to 1.50 Mg/m3 were most affected, specimens compacted to 1.75 Mg/m3 were less affected, while specimens compacted to 2.00 Mg/m3 were unaffected by infiltration of sodium chloride solutions. Variations in dry density of compacted bentonite impacts the pore space available for moisture flow, while, salinity of wetting fluid impacts the pore structure from associated physico-chemical changes in clay structure. Experimental results showed that the unsaturated permeability coefficient is insensitive to variations in dry density and solute concentration of wetting liquid, while, the effective hydraulic diffusivity is impacted by variations in these parameters. Chapter 8 summarises the major findings of the study.

Les études du risque du stockage de déchets radioactifs comprennent, comme toute étude du risque, un traitement de l'incertitude. L'outil de calcul du risque, appelé outil PRA (Probabilistic Risk Assessment), est formé d'un code de calcul d'écoulement des eaux souterraines et de transport de chaînes de radionucléides. Ce type d'outil est essentiel pour l'évaluation de performance de la barrière géologique. Le manque de connaissances au sujet de la variabilité (dans l'espace et le temps) des propriétés hydrogéologiques de cette barrière est la raison primaire de l'incertitude et des méthodes stochastiques ont été développées en hydrogéologie pour le traiter.<p>Dans cette thèse, l'analyse d'incertitude liée à la composition du milieu géologique est partagée entre l'écoulement et le transport de la manière suivante: a) une solution moyenne de l'écoulement est tout d'abord déterminée à l'aide d'un code basé sur la méthode des différences finies. Cette solution est ensuite soumise à une analyse de sensibilité. Cette analyse débouche sur la résolution d'un problème inverse afin d'améliorer l'estimation initiale des paramètres moyens d'écoulement; b) l'effet de la variation aléatoire de la vitesse d'écoulement est envisagé lors du transport des radionucléides. Le transport est résolu à l'aide d'une méthode Monte Carlo non analogue.<p><p>L'analyse de sensibilité du problème d'écoulement est réalisée à l'aide d'une méthode variationnelle. La méthode proposée a comme avantage celui de pouvoir quantifier l'incertitude de structure; c'est-à-dire l'incertitude liée à la géométrie du milieu géologique.<p>Une méthodologie Monte Carlo non analogue est utilisée pour le transport de chaînes de radionucléides en milieu stochastique. Les apports de cette méthodologie pour le calcul du risque reposent sur trois points:<p>1) L'utilisation d'une solution de transport simple (sous la forme d'une solution adjointe) dans les mécanismes de la simulation Monte Carlo. Cette solution de transport permet de résumer, entre deux positions successives du marcheur aléatoire, les processus chimicophysiques (advection, diffusion-dispersion, adsorption, désorption,) apparaissant à l'échelle microscopique. Elle rend possible des simulations efficaces de transport en accélérant les mécanismes de transition des marcheurs aléatoires dans le domaine géologique et dans le temps.<p>2) L'application de la méthode des arbres d'événements continus au transport de chaînes de radionucléides. Cette méthode permet d'envisager les transitions radioactives entre éléments d'une chaîne selon un même formalisme que celui qui prévaut pour les simulations de transport d'un radionucléide unique. Elle permet donc de passer du transport d'un radionucléide au transport d'une chaîne de radionucléides sans coûts supplémentaires en temps de calcul et avec un coût supplémentaire en mémoire limité.<p>3) L'application de techniques dites de "double randomization" au problème de transport de radionucléides dans un milieu géologique stochastique. Ces techniques permettent de combiner efficacement une simulation Monte Carlo de paramètres avec une simulation Monte Carlo de transport et ainsi d'inclure l'incertitude associée à la composition du milieu géologique explicitement dans le calcul du risque.<p><p>Il ressort de ce travail des perspectives prometteuses de développements ultérieurs de la méthodologie Monte Carlo non analogue pour le calcul du risque.<p><p> / Doctorat en sciences appliquées / info:eu-repo/semantics/nonPublished

23000 tonnes de déchets graphites seront générés lors du démantèlement de la première filière de réacteurs en France (9 réacteurs Uranium Naturel Graphite Gas, UNGG). Ces déchets radioactifs sont classés dans la catégorie Faible Activité Vie Longue (FAVL). Dans le cadre de la loi, l’agence nationale pour la gestion des déchets radioactifs (Andra) étudie un concept de stockage à faible profondeur. Cette étude s’intéresse plus particulièrement au carbone 14, qui est un des principaux radionucléides à vie longue (5730 ans) dans les déchets graphite, mais aussi au tritium qui est l’un des principaux contributeurs de la radioactivité à court terme. Ces deux radionucléides ont la particularité d’exister sous différentes formes, aussi bien en phase gaz (14CO2, HT,…) qu’en phase liquide (14CO32-, HTO,…). Leur spéciation va influencer leur migration du stockage vers l’environnement. Des expériences de lixiviation en milieu alcalin (NaOH 0,1mol.L-1, simulant les conditions de stockage), ont été réalisées sur des échantillons de graphites irradiés provenant de deux réacteurs : SLA2 et G2, afin de quantifier leur relâchement et de définir leur spéciation. Les études montrent que le carbone se trouve aussi bien en phase gaz qu’en phase liquide. Dans la phase gaz, le relâchement est faible (< 0,1%), et correspond à des formes oxydables. Le carbone 14 est relâché majoritairement en phase liquide : 65% de la fraction d’inventaire relâchée est sous forme de carbone 14 inorganique, et 35% de carbone 14 organique. Deux formes de tritium ont été identifiées dans la phase gaz : HTO et HT/Tritium Organiquement Lié. Plus de 90% du tritium en phase gaz se trouve sous forme HT/TOL, mais ce relâchement est faible (<0,1%). Majoritairement le tritium est en phase liquide sous forme HTO. / 23000 tons of graphite wastes will be generated during dismantling of the first generation of French reactors (9 gas cooled reactors). These wastes are classified as Long Lived Low Level wastes (LLW-LL). As requested by the law, the French National Radioactive Waste Management Agency (Andra) is studying concepts of low-depth disposals.In this work we focus on carbon 14, the main long-lived radionuclide in graphite waste (5730y), but also on tritium, which is the main contributor to the radioactivity in the short term. Carbon 14 and tritium may be released from graphite waste in many forms in gaseous phase (14CO2, HT…) or in solution (14CO32-, HTO…). Their speciation will strongly affect their migration from the disposal site to the environment. Leaching experiments, in alkaline solution (0.1 M NaOH simulating repository conditions) have been performed on irradiated graphite, from Saint-Laurent A2 and G2 reactors, in order to quantify their release and characterize their speciation. The studies show that carbon 14 exists in both gaseous and aqueous phases. In the gaseous phase, release is weak (<0.1%) and corresponds to oxidizable species. Carbon 14 is mainly released into liquid phase, as both inorganic and organic species. 65% of released fraction is inorganic and 35% organic carbon. Two tritiated species have been identified in gaseous phase: HTO and HT/Organically Bond Tritium. More than 90% of tritium in that phase corresponds to HT/OBT. But release is weak (<0.1%). HTO is mainly in the liquid phase.

Dans le contexte du stockage profond des déchets radioactifs de haute et moyenne activité à vie longue en France, l’argilite de Bure (Arg) a été choisie comme roche hôte notamment pour ses propriétés de rétention des radionucléides. Or, cette roche argileuse dite du Callovo-Oxfordien (COx) contient naturellement de la matière organique (MO). Le but de cette thèse est d’évaluer l’influence de la MO naturelle mobile sur la rétention sur l’argilite de l’europium, analogue classique des actinides trivalents des déchets vitrifiés. Trois molécules organiques sont étudiées : les acides subérique, sorbique et tiglique, acides organiques de faible poids moléculaire identifiés dans l’eau porale naturelle du COx. Toutes les expériences ont été réalisées dans un milieu simulant l’eau du COx (pH=7,5 ; I=0,1 mol/L ; PCO2 =10^(-2) bar).La caractérisation de notre échantillon d’argilite montre sa conformité avec les études précédentes de la zone d’intérêt et que le pH de 7,5 est incontournable pour ne pas dénaturer la roche. L’étude du système Eu-MO montre que les acides organiques n’ont pas d’influence sur la spéciation de l’europium dans l’eau de COx. L’étude expérimentale de l’interaction Eu-Arg confirme que la rétention se fait par sorption sur l’argilite (CEu<6.10-6mol/L) et précipitation dans l’eau de COx (CEu>6.10^(-6)mol/L). Le coefficient de distribution Rd, qui quantifie la sorption, est de 170 ± 30 L/g, valeur élevée conforme aux valeurs documentées sur des argilites naturelles. Enfin, l’étude du système ternaire Eu-MO-Arg montre une légère augmentation de la rétention de Eu en présence de matière organique. Cet effet synergique est très satisfaisant du point de vue de la sûreté du stockage : la présence de ces petits acides organiques naturels ne remet pas en question les propriétés de rétention de l’argilite vis-à-vis de l’europium et des actinides trivalents. / Bure clay rock (CR) was chosen as host rock for the French high and intermediate level long lived radioactive waste repository. This choice is mostly explained by the retention ability of the Callovo-Oxfordian rock (COx). Bure clay rock contains natural organic matter (OM) that could have an influence on radionuclide retention. The aim of this work is to assess the influence of natural mobile OM on the retention of Eu on clay rock. Eu was chosen as a chemical model for trivalent actinides contained in vitrified waste. Three organic molecules were studied: suberic, sorbic and tiglic acids, small organic acids identified in COx pore water. All the experiments were carried out in an environment recreating COx water (pH=7.5 ; I=0.1 mol/L ; PCO2 =10^(-2) bar).Clay rock sample characterization showed that the sample used in this work was similar to those previously extracted from the area of interest and that it was necessary to maintain pH at 7.5 to avoid altering the clay rock. The Eu-OM system study indicated that organic acids had no influence on Eu speciation in COx water. The Eu-CR system experimental study confirmed that retention implied sorption on CR (CEu<6.10^(-6)mol/L) and precipitation in COx water (CEu>6.10-6mol/L). Distribution coefficient Rd (quantifying sorption) was estimated at 170 ± 30 L/g. This high value is consistent with literature values obtained on clay rocks. The ternary Eu-OM-CR system study showed a slight increase of sorption in the presence of organic matter. This synergistic effect is very satisfactory in terms of storage security: the presence of small organic acids in clay rock does not question retention properties with respect to europium and trivalent actinides.

面對高度科技化、工業化及專業化的社會，風險溝通已是政府面對環境爭議時難以規避的課題。回顧台灣近年來各項環境政策所遭遇的激烈抗爭，顯現政府風險溝通的不足。近年來興起的審議式民主，強調在理性與互惠的前提下，讓公民針對議題發表不同意見，成為政府替代傳統風險溝通的另一選項。尤其對於亟需完善風險溝通的高科技議題-「核廢料處置」而言，審議式民主似乎為其帶來契機。本研究透過分析「核廢何從電視公民討論會」審議活動過程政府與民眾的風險溝通關係，以及會議參與者的深度訪談資料，探討審議式會議如何落實風險溝通理念，藉此瞭解並反思審議式民主在台灣的實踐及其能否成為有效的風險溝通機制。 研究發現，在理論層面，審議式民主與風險溝通理論有許多相通之處；而在實踐層面，審議式民主得以落實風險溝通四項核心要素：「雙向互動」、「資訊公開、即時及更新」、「轉譯為常民語言」及「利害關係人參與」；除此之外，與會者及相關人員亦受到審議機制正向的影響；但在此會議中民眾與政府間信任關係的改善程度有限。本研究建議政府未來進行風險溝通時，應健全溝通管道、有效連結「會議結論」與「政策制定」、整合資訊公開管道並縮短數位落差、及處理與核能政策連動問題，方能有助於低放射性廢棄物的風險溝通。 / Risk communication is an unavoidable task when the government faces a highly industrialized and professionalized society. In the past years, environmental policies the government proposed and the protests these policies triggered show the deficiency of the government on risk communication. Recently, the rising deliberative democracy that emphasizes citizen dialogue on the basis of equality, rationality and reciprocity, could become an alternative to traditional risk communication for the government. Especially for the high-tech issue--disposal of nuclear waste-- which is desperate for comprehensive risk communication, deliberative democracy seems to bring the window of opportunity. Through examining the case of “Where Would the Nuclear Waste Go?” TV forum, this study explores risk communication between the government and citizens, and discusses how deliberative forum realizes the idea of risk communication in practice and delivers risk knowledge. Furthermore, this study rethinks the practice of deliberative democracy in Taiwan and accesses whether it could be an effective risk communication mechanism. This study discovers that there is no contradiction between the practice of deliberative forum and the theory of risk communication. Deliberative democracy facilitates four core elements of risk communication: “two-way communication,” “information disclosure, in time and update,” “transfer into the language of ordinary people” and “the participation of stakeholders.” In addition, the participants and staffs were empowered positively by the deliberative mechanism. However, the improvement of trust between the government and citizens is very limited. This study suggests that when conducting risk communication for the low-level radioactive waste issue, the government should enhance risk communication channels, link the conclusions of citizen forums to policy making, integrate various information disclosure mechanisms, bridge the digital divide, and deal with the problem related to the nuclear energy policy.

The chemistry and corrosion mechanisms associated with reduced sulfur compounds such as calcium sulfide, present in ground granulated blast-furnace slag (GGBFS), have been studied in high-density concrete, mortar and simulated pore-water environments. The high-density concrete and mortar samples were produced to replicate the high-density GGBFS concrete, in the dry storage containers (DSCs), used for radiation shielding from used nuclear fuel. Electrochemical measurements on embedded steel electrodes in high-density GGBFS concrete and mortar samples, showed that sulfide is capable of consuming oxygen to create a stable, reducing environment, though not in all cases, and the high-frequency electrolyte resistance increases with hydration time. Ion chromatography on simulated pore-water environments determined that thiosulfate is quite kinetically stable as a sulfide oxidation product and magnetite is capable of oxidizing sulfide. Microscopy has also been used to provide visual evidence of GGBFS hydration and elemental quantification of the hydrating microstructure in different environments.

The chemistry and corrosion mechanisms associated with reduced sulfur compounds such as calcium sulfide, present in ground granulated blast-furnace slag (GGBFS), have been studied in high-density concrete, mortar and simulated pore-water environments. The high-density concrete and mortar samples were produced to replicate the high-density GGBFS concrete, in the dry storage containers (DSCs), used for radiation shielding from used nuclear fuel. Electrochemical measurements on embedded steel electrodes in high-density GGBFS concrete and mortar samples, showed that sulfide is capable of consuming oxygen to create a stable, reducing environment, though not in all cases, and the high-frequency electrolyte resistance increases with hydration time. Ion chromatography on simulated pore-water environments determined that thiosulfate is quite kinetically stable as a sulfide oxidation product and magnetite is capable of oxidizing sulfide. Microscopy has also been used to provide visual evidence of GGBFS hydration and elemental quantification of the hydrating microstructure in different environments.

The purpose of the work described in this thesis was to explore the use of fractional crystallization as a technology that can be used to separate medium-curie waste from the Hanford Site tank farms into a high-curie waste stream, which can be sent to a Waste Treatment and Immobilization Plant (WTP), and a low-curie waste stream, which can be sent to Bulk Vitrification. The successful semi-batch crystallization of sodium salts from two single shell tank simulant solutions (SST Early Feed, SST Late Feed) demonstrated that the recovered crystalline product met the purity requirement for exclusion of cesium, sodium recovery in the crystalline product and the requirement on the sulfate-to-sodium molar ratio in the stream to be diverted to the WTP. The experimental apparatus, procedures and results obtained in this thesis on scaled-down experiments of SST Early and Late Feed simulated solutions were adapted and reproduced under hot-cell with actual wastes by our partners at Hanford. To prepare the application of the pretreatment process to pilot scale process, several varation to the feed solutions were investigated including the presence of carboxylates and amines organics compounds and solids particles. Results of the study showed that 4 organics species presented complications to the process (NTA, HEDTA, EDTA and sodium citrate) while the other species (Formate, acetate, glycolate and IDA) and solids particles did not in the conditions of the stored wastes. In this thesis, the kinetics of the crystalline species formed at the condition of the early feed certification run (66 °C and 25 g/h evaporation) were determined along with the effect of the operating temperature and evaporation rate on these kinetics. On one hand, the study of evaporation rate values ranging from 25g/h to 75g/h showed that an increase in evaporation rate increased the specific nucleation while decreasing the specific growth rate. On the other hand, experiments on operating temperature ranging from 35 °C to 75 °C displayed that the nucleation rate of all species increased with temperature at the exception of sodium carbonate monohydrate and burkeite crystals, and that the growth rate of all species increased with temperature at the exception of sodium nitrate. Furthermore, sulfate based crystals such as trisodium fluoride sulfate were only roduced at 45 °C and 75 °C. A simple steady state MSMPR population balance model was developed expressing the total population density function as the sum of the specific population density functions. The specific semi-batch crystallization kinetics were implemented in this model.