Pluri-millenial evolution of uranium speciation in lacustrine sediments

2020 ◽  
Author(s):  
Pierre Lefebvre ◽  
Alkiviadis Gourgiotis ◽  
Arnaud Mangeret ◽  
Pierre Le Pape ◽  
Olivier Diez ◽  
...  
Keyword(s):  
Contaminated Soils ◽  
Sediment Cores ◽  
Lacustrine Sediments ◽  
Storage Conditions ◽  
Edge Structure ◽  
Anoxic Conditions ◽  
X Ray ◽  
Long Term Storage ◽  
X Ray Absorption

<p>Uranium (U) is a toxic radionuclide which environmental dissemination must be limited. In this regard, understanding U immobilization mechanisms in reducing environments is essential for improving the management of radioactive waste and the remediation of contaminated sites. In particular, determining the long-term behavior of non-crystalline U(IV) species in (sub-)surface conditions is of growing importance, as these environmentally-relevant species have been recently showed to play a major role in U mobility. For this purpose, we investigated the evolution of U speciation over a pluri-millennial period in naturally U-enriched sediments from Lake Nègre (alt. 2354 m, Mercantour, France) as an analogue of contaminated systems. Several sediment cores were sampled at 24 m of water depth and preserved under anoxic conditions. Bottom sediments were dated back to 8700 cal BP. These organic- and Si-rich sediments display increasing U concentration with depth, from 350 to more than 1000 µg/g. Sequential ultrafiltration of surface waters and uranium isotopic ratios (<sup>238</sup>U/<sup>235</sup>U and (<sup>234</sup>U/<sup>238</sup>U)) of sediments and waters suggest that the deposition mode of U did not vary significantly with time, thus giving the opportunity to follow the effect of diagenesis on U speciation over more than 1000 years. Uranium L<sub>III</sub>-edge X-Ray Absorption Near-Edge Structure (XANES) analysis shows that U is rapidly reduced in the upper sediment layers and is fully reduced at depth. Preliminary Extended X-Ray Absorption Fine Structure (EXAFS) spectroscopy data at the U L<sub>III</sub>-edge reveals that U speciation evolved with depth in the sediment core, suggesting an effect of diagenesis in anoxic conditions on U solid speciation. Our results may help to design long-term storage conditions that are able to enhance the formation of poorly soluble U species in U-contaminated soils and sediments.</p>

scholarly journals Biomineralization of Cu2S Nanoparticles by Geobacter sulfurreducens

2020 ◽  
Vol 86 (18) ◽  
Author(s):  
Richard L. Kimber ◽  
Heath Bagshaw ◽  
Kurt Smith ◽  
Dawn M. Buchanan ◽  
Victoria S. Coker ◽  
...  
Keyword(s):  
Biogeochemical Cycling ◽  
Geobacter Sulfurreducens ◽  
Edge Structure ◽  
Colloidal Transport ◽  
Content Type ◽  
Anoxic Conditions ◽  
X Ray ◽  
Sulfate Reducing ◽  
Wide Range ◽  
X Ray Absorption

ABSTRACT Biomineralization of Cu has been shown to control contaminant dynamics and transport in soils. However, very little is known about the role that subsurface microorganisms may play in the biogeochemical cycling of Cu. In this study, we investigate the bioreduction of Cu(II) by the subsurface metal-reducing bacterium Geobacter sulfurreducens. Rapid removal of Cu from solution was observed in cell suspensions of G. sulfurreducens when Cu(II) was supplied, while transmission electron microscopy (TEM) analyses showed the formation of electron-dense nanoparticles associated with the cell surface. Energy-dispersive X-ray spectroscopy (EDX) point analysis and EDX spectrum image maps revealed that the nanoparticles are rich in both Cu and S. This finding was confirmed by X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analyses, which identified the nanoparticles as Cu2S. Biomineralization of CuxS nanoparticles in soils has been reported to enhance the colloidal transport of a number of contaminants, including Pb, Cd, and Hg. However, formation of these CuxS nanoparticles has only been observed under sulfate-reducing conditions and could not be repeated using isolates of implicated organisms. As G. sulfurreducens is unable to respire sulfate, and no reducible sulfur was supplied to the cells, these data suggest a novel mechanism for the biomineralization of Cu2S under anoxic conditions. The implications of these findings for the biogeochemical cycling of Cu and other metals as well as the green production of Cu catalysts are discussed. IMPORTANCE Dissimilatory metal-reducing bacteria are ubiquitous in soils and aquifers and are known to utilize a wide range of metals as terminal electron acceptors. These transformations play an important role in the biogeochemical cycling of metals in pristine and contaminated environments and can be harnessed for bioremediation and metal bioprocessing purposes. However, relatively little is known about their interactions with Cu. As a trace element that becomes toxic in excess, Cu can adversely affect soil biota and fertility. In addition, biomineralization of Cu nanoparticles has been reported to enhance the mobilization of other toxic metals. Here, we demonstrate that when supplied with acetate under anoxic conditions, the model metal-reducing bacterium Geobacter sulfurreducens can transform soluble Cu(II) to Cu2S nanoparticles. This study provides new insights into Cu biomineralization by microorganisms and suggests that contaminant mobilization enhanced by Cu biomineralization could be facilitated by Geobacter species and related organisms.

Solid-phase speciation of Zn in road dust sediment

2011 ◽  
Vol 75 (5) ◽  
pp. 2611-2629 ◽  
Author(s):  
J. E. S. Barrett ◽  
K. G. Taylor ◽  
K. A. Hudson-Edwards ◽  
J. M. Charnock
Keyword(s):  
Solid Phase ◽  
Road Dust ◽  
Edge Structure ◽  
X Ray ◽  
Urban Road ◽  
Hydrous Oxides ◽  
Increased Risk ◽  
Soluble Species ◽  
X Ray Absorption

AbstractX-ray absorption spectroscopy, scanning electron microscopy (SEM) and X-ray diffractometry (XRD) have been used to study the solid-phase speciation of Zn in urban road dust sediments (RDS) in Manchester, UK. X-ray absorption near-edge structure (XANES) analysis using linear combination modelling suggest that the soluble species Zn(NO3)2·6H2O and ZnCl2 represent 70—83%, and Zn-sorbed goethite 17—30%, of the Zn species present. The presence of goethite is not corroborated by extended X-ray absorption fine structure (EXAFS) modelled first shell scattering Zn—O distances of 2.01—2.03 Å, but this may be due to distortion of the Zn octahedra on the goethite surface, or the existence of Zn-sorbed species with other metal hydrous oxides, as inferred by the EXAFS-modelled second shell Fe and Al scatterers. Analysis by EXAFS also suggests that metallic Zn-Cu-Sn-Pb and Zn-silicate phases are present in the RDS, and this is corroborated by SEM and XRD. Other phases suggested by EXAFS include ZnO, franklinite, Zn-sorbed birnessite and zinc formate. Differences between the XANES and other results suggest that model compounds such as Zn-bearing phyllosilicates and metallic Zn phases may have been missing from the XANES fitting. Long-term low-level exposure to the RDS Zn phases identified may lead to an increased risk of cardiovascular or pulmonary diseases.

scholarly journals Tc and Re Behavior in Borosilicate Waste Glass Vapor Hydration Tests

2006 ◽  
Vol 985 ◽  
Author(s):  
David A. McKeown ◽  
Andrew C. Buechele ◽  
Wayne W. Lukens ◽  
David K. Shuh ◽  
Ian L. Pegg
Keyword(s):  
High Mobility ◽  
Sample Surface ◽  
Hydrothermal Conditions ◽  
X Ray ◽  
Long Term Storage ◽  
Before And After ◽  
X Ray Absorption ◽  
Term Storage ◽  
Scanning Electron

AbstractTechnetium (Tc), found in some nuclear wastes, is of particular concern with regard to long-term storage, because of its long-lived radioactivity and high mobility in the environment. Tc and rhenium (Re), commonly used as a non-radioactive surrogate for Tc, were studied to assess their behavior in borosilicate glass under hydrothermal conditions in the Vapor Hydration Test (VHT). X-ray absorption spectroscopy (XAS) and scanning electron microscopy (SEM) measurements were made on the original Tc- and Re-containing glasses and their corresponding VHT samples, and show different behavior for Tc and Re under VHT conditions. XAS indicates that, despite starting with different Tc(IV) and Tc(VII) distributions in each glass, the VHT samples have 100% Tc(IV)O6 environments. SEM shows complete alteration of the original glass, Tc enrichment near the sample surface, and Tc depletion in the center. Perrhenate (Re(VII)O4−) is dominant in both Re-containing samples before and after the VHT, where Re is depleted near the VHT sample surface and more concentrated toward the center.

Preparation And elemental analysis of ancient fibers

1987 ◽  
Vol 45 ◽  
pp. 410-411
Author(s):  
Allen Angel ◽  
Kathryn A. Jakes
Keyword(s):  
Cross Sections ◽  
Physical Structure ◽  
Energy Dispersive ◽  
Archaeological Sites ◽  
X Ray ◽  
Long Term Storage ◽  
Backscattered Electron ◽  
Electron Imaging

Fabrics recovered from archaeological sites often are so badly degraded that fiber identification based on physical morphology is difficult. Although diagenetic changes may be viewed as destructive to factors necessary for the discernment of fiber information, changes occurring during any stage of a fiber's lifetime leave a record within the fiber's chemical and physical structure. These alterations may offer valuable clues to understanding the conditions of the fiber's growth, fiber preparation and fabric processing technology and conditions of burial or long term storage (1).Energy dispersive spectrometry has been reported to be suitable for determination of mordant treatment on historic fibers (2,3) and has been used to characterize metal wrapping of combination yarns (4,5). In this study, a technique is developed which provides fractured cross sections of fibers for x-ray analysis and elemental mapping. In addition, backscattered electron imaging (BSI) and energy dispersive x-ray microanalysis (EDS) are utilized to correlate elements to their distribution in fibers.

Chemical and orientational imaging of polymeric samples

1994 ◽  
Vol 52 ◽  
pp. 68-69
Author(s):  
H. Ade ◽  
B. Hsiao ◽  
G. Mitchell ◽  
E. Rightor ◽  
A. P. Smith ◽  
...  
Keyword(s):  
Ethylene Terephthalate ◽  
National Laboratory ◽  
Brookhaven National Laboratory ◽  
Carbonyl Groups ◽  
Aromatic Rings ◽  
Edge Structure ◽  
X Ray ◽  
Scanning Transmission ◽  
Polymeric Samples ◽  
X Ray Absorption

We have used the Scanning Transmission X-ray Microscope at beamline X1A (X1-STXM) at Brookhaven National Laboratory (BNL) to acquire high resolution, chemical and orientation sensitive images of polymeric samples as well as point spectra from 0.1 μm areas. This sensitivity is achieved by exploiting the X-ray Absorption Near Edge Structure (XANES) of the carbon K edge. One of the most illustrative example of the chemical sensitivity achievable is provided by images of a polycarbonate/pol(ethylene terephthalate) (70/30 PC/PET) blend. Contrast reversal at high overall contrast is observed between images acquired at 285.36 and 285.69 eV (Fig. 1). Contrast in these images is achieved by exploring subtle differences between resonances associated with the π bonds (sp hybridization) of the aromatic groups of each polymer. PET has a split peak associated with these aromatic groups, due to the proximity of its carbonyl groups to its aromatic rings, whereas PC has only a single peak.

In Vivo Investigation of the Distribution and the Local Speciation of Selenium inAlliumcepa L. by Means of Microscopic X-ray Absorption Near-Edge Structure Spectroscopy and Confocal Microscopic X-ray Fluorescence Analysis

2006 ◽  
Vol 78 (22) ◽  
pp. 7616-7624 ◽  
Author(s):  
Ewa Bulska ◽  
Irena A. Wysocka ◽  
Małgorzata H. Wierzbicka ◽  
Kristof Proost ◽  
Koen Janssens ◽  
...  
Keyword(s):  
Fluorescence Analysis ◽  
Edge Structure ◽  
X Ray ◽  
X Ray Absorption

Full-Field Calcium K-Edge X-ray Absorption Near-Edge Structure Spectroscopy on Cortical Bone at the Micron-Scale: Polarization Effects Reveal Mineral Orientation

2016 ◽  
Vol 88 (7) ◽  
pp. 3826-3835 ◽  
Author(s):  
Bernhard Hesse ◽  
Murielle Salome ◽  
Hiram Castillo-Michel ◽  
Marine Cotte ◽  
Barbara Fayard ◽  
...  
Keyword(s):  
Cortical Bone ◽  
Edge Structure ◽  
Full Field ◽  
Polarization Effects ◽  
X Ray ◽  
X Ray Absorption

scholarly journals Database of ab initio L-edge X-ray absorption near edge structure

2021 ◽  
Vol 8 (1) ◽  
Author(s):  
Yiming Chen ◽  
Chi Chen ◽  
Chen Zheng ◽  
Shyam Dwaraknath ◽  
Matthew K. Horton ◽  
...  
Keyword(s):  
High Throughput ◽  
Scattering Theory ◽  
Research Community ◽  
Metal Compounds ◽  
Edge Structure ◽  
X Ray ◽  
Initial Release ◽  
Computational Workflow ◽  
X Ray Absorption

AbstractThe L-edge X-ray Absorption Near Edge Structure (XANES) is widely used in the characterization of transition metal compounds. Here, we report the development of a database of computed L-edge XANES using the multiple scattering theory-based FEFF9 code. The initial release of the database contains more than 140,000 L-edge spectra for more than 22,000 structures generated using a high-throughput computational workflow. The data is disseminated through the Materials Project and addresses a critical need for L-edge XANES spectra among the research community.

scholarly journals Co-encapsulation of vegetable oils with phenolic antioxidants and evaluation of their oxidative stability under long-term storage conditions

LWT ◽  
2021 ◽  
Vol 142 ◽  
pp. 111033
Author(s):  
Lorine Le Priol ◽  
Justine Gmur ◽  
Aurélien Dagmey ◽  
Sandrine Morandat ◽  
Karim El Kirat ◽  
...  
Keyword(s):  
Oxidative Stability ◽  
Vegetable Oils ◽  
Storage Conditions ◽  
Phenolic Antioxidants ◽  
Long Term Storage ◽  
Term Storage
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