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Mécanismes d’interaction du nickel et de l´europium avec la calcite / Interaction mechanisms of europium and nickel with calciteSabau, Andrea 27 March 2015 (has links)
Dans le contexte de l’évaluation de la sûreté d’un stockage de déchets radioactifs en site géologique profond, les réactions de sorption sont un des principaux processus à prendre en compte pour prédire la migration des radionucléides. Ce travail est axé sur deux éléments: l´Eu(III) comme analogue des certains actinides trivalents et le Ni(II) en tant que produit d’activation. La calcite a été choisie comme solide d´étude en tant que composant des argilites du Callovo-Oxfordien. Notre étude combine des expériences de type batch avec des techniques spectroscopiques (SLRT, RBS et MEB-EDXS) pour élucider les mécanismes qui se produisent à l’interface Eu(III) / Ni(II) – calcite. Pour obtenir une meilleure compréhension des systèmes, avant de commencer les expériences de sorption, la chimie en solution de l’Eu(III) et du Ni(II) a été systématiquement étudiée. La calcite a montré une forte rétention de l'Eu(III), quelle que soit la concentration initiale, le temps de contact et la pression partielle de CO2. Ni(II) est également aisément retenu par la calcite, mais la rétention est dépendante de ces deux paramètres. Les résultats de désorption indiquent une réversibilité partielle pour Ni(II). La SLRT a montré l’influence de la concentration et du temps de contact sur l’interaction de l’Eu(III) avec la calcite. Avec l’aide de la RBS et de la MEB/EDX, elle a permis de discriminer entre différents mécanismes tels que la précipitation de surface, la formation de complexes de surface de sphère interne et l'incorporation. La RBS a démontré l'incorporation de l'Eu(III) dans la calcite jusqu’à une profondeur de 250 nm, contrairement au Ni(II) qui lui reste situé en surface. / In the context of the safety assessment of an underground repository for nuclear waste, sorption reactions are one of the main processes to take into account to predict the migration of the radionuclides. This work is focused on two elements: Eu(III) as an analogue of trivalent actinides and Ni(II) as activation product. Calcite was chosen as adsorbent due to its presence in Callovian-Oxfordian argillites. Our study combines batch experiments with spectroscopic techniques (TRLFS, RBS and SEM-EDXS) to elucidate the mechanisms occurring at Eu(III)/Ni(II) calcite interface. To obtain a better understanding on the systems, before starting sorption experiments, aqueous chemistry of Eu(III) and Ni(II) was carefully investigated. Macroscopic results showed a strong retention of Eu(III) on calcite, no matter the initial concentration, contact time and CO2 partial pressure. Ni(II) was also readily sorbed by calcite, but the retention was influenced by contact time and concentration. Time-dependent sorption experiments showed a marked and slow increase of retention upon a long time range (up to 4 months).Desorption results indicated a partly reversible sorption for Ni(II). TRLFS highlighted the influence of initial concentration and contact time on the interaction of Eu(III) with calcite. With the help of RBS and SEM-EDXS, it enabled to discriminate between different mechanisms like surface precipitation, inner-sphere complexation and incorporation. RBS showed incorporation of Eu(III) into calcite up to 250 nm, contrary to Ni(II) which was located at the surface.
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The First 40Ar/39Ar Ages and Tephrochronologic Framework for the Jurassic Entrada Sandstone in central UtahDossett, Toby S. 01 May 2014 (has links) (PDF)
The first 40Ar/39Ar ages of the Middle Jurassic Entrada Sandstone were derived from tephra beds found in central Utah. Eight air fall ash beds in the Entrada Sandstone, with 40Ar/39Ar biotite ages ranging from 168.1 ± 0.2 to 160.8 ± 0.2 Ma, help to establish the age of Entrada deposition. They were also used to create the first chronostratigraphic divisions within the mudstone-dominated Entrada Sandstone. Statistical cluster analysis of chemical data from electron microprobe analyses of phenocrysts were used as a second line of evidence to test absolute age and stratigraphic correlations. The first direct correlations of two distinct air fall ash beds within Jurassic rocks were correlated using three criteria: (1) stratigraphic position, (2) absolute ages, and (3) mineral chemistry. These tephra beds were identified and correlated across significant lateral distances (~40 km) of the San Rafael Swell in central Utah, and one can be correlated farther southwest to Cannonville, Utah (~160 km) using absolute age relationships. This latter tephra bed allows for stratigraphic correlation across significant facies and thickness changes thereby establishing a regional framework that future studies can use to make more accurate and precise litho- and sequence stratigraphic correlations. Absolute ages from a tephra bed ~20 m below the J-3 unconformity provide a lower age boundary for formation of the J-3 surface. Mega- and microfossil assemblages in the overlying Curtis Formation together with the radiometric ages reported in this study indicate that the age of the Callovian-Oxfordian boundary in the 2004 geologic time scale (161.2 ± 4.0 Ma) is more correct than the current boundary age (163.5 ± 1.1 Ma) in the 2012 geologic time scale.
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Sedimentology and Stratigraphy of the Middle Jurassic Preuss Sandstonein Northern Utah and Eastern IdahoCook, Preston Scott 01 June 2016 (has links)
The purpose of this study is to analyze the sedimentology and stratigraphy of the Middle Jurassic Preuss Sandstone and re-evaluate past sedimentological interpretations. The Preuss is located in northern Utah, western Wyoming and eastern Idaho and is stratigraphically equivalent to the Entrada Sandstone, which is Callovian in age (Dossett et al., 2014). This study is the first attempt at 1) a sequence stratigraphic framework, 2) a petroleum system analysis and 3) an extraterrestrial analog study for the Preuss. This study frames the Preuss within three broad facies groups: marine, coastal and terrestrial. The marine group includes the open marine and restricted marine facies with associated subfacies, the coastal group includes coastal sabkha and associated subfacies, and the terrestrial group includes alluvial, inland sabkha and eolian facies with associated subfacies. Three sections in northern Utah and one section in eastern Idaho compromise the focus of this study. The three Utah sections were measured and described, and samples were collected from two Utah sections and the Idaho section. The Preuss Sandstone was deposited in an asymmetrical retroarc basin, consequently the Preuss thickens from the east towards west-central Utah and the Jurassic Elko highlands. The deposits are mostly terrestrial, which is in accord with recent sedimentological interpretations, but at odds with the old paradigm, which postulates that the Entrada and Preuss were largely tidal in origin. There are marine transgressions within the trough of the retroarc basin, and the transgressions affect terrestrial sedimentary patterns. During marine incurstions, alluvium shed off the highlands is confined west of the seaway, and does not prograde east of the trough until all the available accommodation is filled. The Preuss was deposited during a complete third-order sequence-stratigraphic cycle that lies within the Lower Zuni II second-order lowstand. The Preuss Sandstone can be used as an outcrop analog for ancient and modern environments both here on Earth and on other planetary bodies. The petroliferous Norphlet Formation along the U.S. Gulf Coast was deposited in an environment very similar to the Preuss, but the Waltherian succession of facies might be slightly different. Likewise, the facies present in the Preuss are analogous to modern arid environments, such as the Persian Gulf. Furthermore, the alluvial, sabkha, eolian and shallow marine facies of the Preuss are highly similar to facies observed in ancient Martian environments and modern environments on Saturn's moon, Titan.
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Facies Analysis, Sequence Stratigraphy and Paleogeography of the Middle Jurassic (Callovian) Entrada Sandstone: Traps, Tectonics, and AnalogJennings, George R., III 05 June 2014 (has links) (PDF)
The late Middle Jurassic (Callovian) Entrada Sandstone has been divided into two general facies associations consisting primarily of eolian sandstones in eastern Utah and "muddy" redbeds in central Utah. Sedimentary structures within the redbed portion are explained by the interfingering of inland sabkha, alluvial, and eolian depositional systems. A complete succession from the most basinward facies to the most terrestrial facies in the Entrada Sandstone consists of inland sabkha facies overlain by either alluvial or eolian facies. Where both alluvial and eolian facies interfinger, alluvial facies overlain by eolian facies is considered a normal succession. Sequence boundaries, often identified by more basinward facies overlying more landward facies, are observed in the Entrada Sandstone and are extrapolated for the first time across much of Utah, including both the eolian-dominated and redbed-dominated areas. Using these sequence boundaries as well as recent tephrochronologic studies, three time correlative surfaces have been identified in the Entrada. Based on the facies interpretations at each surface, five paleogeographic reconstructions and five isopach maps have been created, illustrating two major intervals of erg expansion and the location of the Jurassic retroarc foreland basin's potential forebulge. Eolian (erg-margin) sandstones pinch-out into muddy redbeds creating combination traps, as evidenced by dead oil (tar) and bleached eolian sandstone bodies within the Entrada. The Entrada Sandstone is a world-class analog for similar systems, such as the Gulf of Mexico's Norphlet Sandstone, where eolian facies grade into muddy redbed facies.
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