Materials science: displaced by radiation.
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Biomedical subjects
Publications and source records attributed to Rodney C Ewing.
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Sorption of actinides, particularly plutonium, onto submicrometer-sized colloids increases their mobility, but these plutonium colloids are difficult to detect in the far-field. We identified actinides on colloids in the groundwater from the Mayak Production Association, Urals, Russia; at the source, the plutonium activity is approximately 1000 becquerels per liter. Plutonium activities are still 0.16 becquerels per liter at a distance of 3 kilometers, where 70 to 90 mole percent of the plutonium is sorbed onto colloids, confirming that colloids are responsible for the long-distance transport of plutonium. Nano-secondary ion mass spectrometry elemental maps reveal that amorphous iron oxide colloids adsorb Pu(IV) hydroxides or carbonates along with uranium carbonates.
Time-resolved laser-induced fluorescence spectroscopy (TRLFS) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) were applied to investigate the species of uranyl(VI) adsorbed onto muscovite platelets and muscovite suspensions (grain size: 63-200 microm). TRLFS provided evidence for the presence of two adsorbed uranium(VI) surface species on edge-surfaces of muscovite. The two species showed different positions of the fluorescence emission bands and different fluorescence lifetimes indicating a different coordination environment for the two species. HAADF-STEM revealed that nanoclusters of an amorphous uranium phase were attached to the edge-surfaces of muscovite powder during batch sorption experiments. These U-nanoclusters were not observed on {00/} cleavage planes of the muscovite. The surface species with the shorter fluorescence lifetimes are interpreted as truly adsorbed bidentate surface complexes, in which the U(VI) binds to aluminol groups of edge-surfaces. The surface species with the longer fluorescence lifetimes are interpreted to be an amorphous U(VI) condensate or nanosized clusters of polynuclear uranyl(VI) surface species with a particle diameter of 1 to 2 nm. Depending on the size of these clusters the fluorescence lifetimes vary; i.e., the larger the nanosized clusters, the longer is the fluorescence lifetime.
Small-angle light scattering is used to assess the dispersion behavior of vapor-grown carbon nanofibers suspended in water. These data provide the first insights into the mechanism by which surface treatment promotes dispersion. Both acid-treated and untreated nanofibers exhibit hierarchical morphology consisting of small-scale aggregates (small bundles) that agglomerate to form fractal clusters that eventually precipitate. Although the morphology of the aggregates and agglomerates is nearly independent of surface treatment, their time evolution is quite different. The time evolution of the small-scale bundles is studied by extracting the size distribution from the angle-dependence of the scattered intensity, using the maximum entropy method in conjunction with a simplified tube form factor. The bundles consist of multiple tubes possibly aggregated side-by-side. Acid oxidation has little effect on this bundle morphology. Rather acid treatment inhibits agglomeration of the bundles. The time evolution of agglomeration is followed by fitting the scattering data to a generalized fractal model. Agglomerates appear immediately after cessation of sonication for untreated fibers but only after hours for treated fibers. Eventually, however, both systems precipitate.
Exposure to airborne particulates containing low concentrations of heavy metals, such as Pb, As, and Se, may have serious health effects. However, little is known about the speciation and particle size of these airborne metals. Fine- and ultrafine particles with heavy metals in aerosol samples from the Detroit urban area, Michigan, were examined in detail to investigate metal concentrations and speciation. The characterization of individual particles was completed using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with conventional high-resolution TEM techniques. The trace elements, Pb, As, La, Ce, Sr, Zn, Cr, Se, Sn, Y, Zr, Au, and Ag, were detected, and the elemental distributions were mapped in situ atthe nanoscale. The crystal structures of the particles containing Pb, Sr, Zn, and Au were determined from their electron diffraction patterns. Based on the characterization of the representative trace element particles, the potential health effects are discussed. Most of the trace element particles detected in this study were within a range of 0.01-1.0 microm in size, which has the longest atmospheric residence time (approximately 100 days). Increased chemical reactivity owing to the size of nanoparticles may be expected for most of the trace metal particles observed.
A major challenge to the development of a fundamental understanding of transport and retardation mechanisms of trace metal contaminants (<10 ppm) is their identification and characterization at the nanoscale. Atomic-scale techniques, such as conventional transmission electron microscopy, although powerful, are limited by the extremely small amounts of material that are examined. However, recent advances in electron microscopy provide a number of new analytical techniques that expand its application in environmental studies, particularly those concerning heavy metals on airborne particulates or water-borne colloids. High-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), STEM-energy-dispersive X-ray spectrometry (EDX), and energy-filtered TEM (EFTEM) can be effectively used to identify and characterize nanoparticles. The image contrast in HAADF-STEM is strongly correlated to the atomic mass: heavier elements contribute to brighter contrast. Gold nanocrystals in pyrite and uranium nanocrystals in atmospheric aerosols have been identified by HAADF-STEM and STEM-EDX mapping and subsequently characterized by high-resolution TEM (HRTEM). EFTEM was used to identify U and Fe nanocrystals embedded in an aluminosilicate. A rare, As-bearing nanophase, westerveldite (FeAs), was identified by STEM-EDX and HRTEM. The combined use of these techniques greatly expands the effective application of electron microscopy in environmental studies, especially when applied to metals of very low concentrations. This paper describes examples of how these electron microbeam techniques can be used in combination to characterize a low concentration of heavy metals (a few ppm) on nanoscale particles.
Particulates emitted from coal-burning power plants typically contain very small amounts of uranium (<10 ppm). Because of the extremely low concentrations, the form of the uranium has been unknown. Using a variety of advanced electron microscopy techniques, we have identified for the first time nanocrystals of uraninite, UO2+x, encapsulated in carbonaceous matter (< or = 50 nm) similar to fullerene. We have also identified, for the first time, closely associated fullerenes, C60. The "carbon-caged" nanocrystals of uraninite are protected from the immediate oxidation that would lead to increased mobility of uranium in the environment. Still, the presence of uranium in the very fine fraction of atmospheric particulates provides another pathway for radiation exposure.
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