Download EBOOK Uranium and Strontium (Bio)Geochemistry: Limits on Uranium and Strontium Mobility in the Environment PDF for free


Download EBOOK Uranium and Strontium (Bio)Geochemistry: Limits on Uranium and Strontium Mobility in the Environment PDF for free Category: Science & Geography
The author of the book: David Marc Singer
Format files: PDF, EPUB, TXT, DOCX
The size of the: 7.12 MB
Language: English
ISBN-13: 9781243552396
Edition: Proquest, Umi Dissertation Publishing
Date of issue: 1 September 2011

Description of the book "Uranium and Strontium (Bio)Geochemistry: Limits on Uranium and Strontium Mobility in the Environment":

This dissertation examines specific (bio)geochemical aspects of U sequestration processes at the applied and fundamental levels using a combination batch sorption experiments, a suite of bulk and particle surface characterization techniques, and synchrotron-based X-ray spectroscopic and diffraction techniques. Uranium speciation and distribution have been determined in contaminated vadose and groundwater zone sediments from the Hanford, Washington 300 Area Process Pond site. We used synchrotron-based micro-X-ray fluorescence (muXRF) imaging, micro-X-ray absorption near edge structure (muXANES) spectroscopy, and micro-X-ray diffraction (muXRD) techniques combined with bulk U L III-edge EXAFS spectroscopy to determine the distribution PDF and speciation of U and Cu through the vadose and groundwater zones beneath North Process Pond #2. muXRF imaging, muXRD, and muXANES spectroscopy revealed two major U occurrences within the vadose and groundwater zones: (1) low to moderate concentrations of U(VI) associated with mineral surfaces (particularly chlorite), and (2) U(VI) hotspots consisting of micron-sized particles associated with surface coatings on grains of muscovite and chlorite, spatially correlated with Cu(II) hotspots. In the groundwater zone, these particles were identified as cuprosklodowskite and metatorbernite. In contrast, the U-Cu-containing particles are X-ray amorphous in the vadose ePub zone. Analyses of U LIII -edge XAFS spectra by linear-combination fitting indicate that U speciation consists of ∼75% uranyl sorbed to clays and ∼25% metatorbernite-like X-ray amorphous U-Cu-phosphates (middle vadose zone), nearly 100% sorbed uranyl (lower vadose zone), and ∼70% sorbed uranyl and ∼30% cuprosklodowskite/metatorbernite (ground water zone). These findings suggest that dissolution of U(VI)-Cu(II)-bearing solids as well as desorption of U(VI), mainly from phyllosilicates, are important sources of U(VI) in the Area 300 groundwater plume. Future subsurface transport of U released from the 300 Area sediments and similar PDF sites will be strongly affected by uranium adsorption to subsurface materials, particularly clay minerals which can be a major sink for U in contaminated environments. We have used a series of batch sorption/desorption experiments combined with U LIII-edge X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopy and surface complexation modeling to investigate the dominant sorption process(es) governing uranyl uptake by chlorite. Sorption was independent of ionic strength, suggesting a dominantly inner-sphere sorption mechanism. The maximum sorption loading was 0.28 mumoles U g-1 chlorite at pH 4, whereas the maximum sorption loading ePub was 6.3 mumoles U g-1 chlorite at pH 6.5 and pH 10. U(VI) uptake was also dependent on the solution composition, i.e., the presence of CO3 and Ca. A desorption experiment performed as a series of sequential extraction steps indicated that (1) there is little or no weakly bound U(VI) or U(VI) coprecipitated with ferrihydrite, (2) 60 to 80% of U(VI) inner-sphere sorption complexes are desorbed following a 0.1 M HCl step over one week, and (3) 100% desorption of adsorbed U(VI) is accomplished by a 1.0 M HCl step over one week. Fits of the U LIII-edge EXAFS spectra of PDF short-term sorption samples indicate that U(VI) forms inner-sphere sorption complexes at [Fe(O, OH)6] octahedral sites in a bidentate manner, with evidence for U(VI)-CO3 sorption complexes were present, although there was no evidence for U(VI)-CO3-Ca sorption complexes. The EXAFS-derived parameters were used to constrain the type(s) of U(VI)-bearing surface...

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Download EBOOK Uranium and Strontium (Bio)Geochemistry: Limits on Uranium and Strontium Mobility in the Environment PDF for free



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