Microanalysis of Heterogeneous Radiation in Particulate Matter as an Aid to Nuclear Source Identification

Kaltofen, Marco Paul Johann

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Microanalysis of Heterogeneous Radiation in Particulate Matter as an Aid to Nuclear Source Identification

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Radionuclides in particulate matter associated with outdoor and indoor dusts were analyzed to determine the form and concentration of radioactive isotopes present. These radioactive isotopes, such as Strontium 90, Cesium 137, and Uranium 235, consist of, or are sorbed onto fine particulate matter, (PM). The airborne dispersion of this fine particulate matter results in the facilitated transport of these sorbed or neat radionuclides. Sources of particulate-bound radioactive contaminants include fallout from weapons testing, accumulation of radon daughters, transport of soils containing naturally-occurring radioactive material, remediation of radiologically-contaminated sites, and nuclear material processing. Radiological contaminants in PM, may exist as trace contamination in homogenous collections of particles, but may also exist heterogeneously, as a small number of high-concentration radionuclides among a larger set of uncontaminated particles. A total of 114 samples of indoor and outdoor airborne dusts were collected from a former nuclear weapons production facility near Richland, WA, the Los Alamos National Laboratory, and the Yakama Indian Nation in Wapato, WA. Los Alamos, NM was also the site of the May 2000 Cerro Grande wildfire. The wildfire created very large amounts of airborne particulate matter, including smoke and soot. The area affected by open burning included 43,000 acres. At the national laboratory, greater than 7600 acres were affected, including some areas that were radiologically- contaminated, such as a U-238 ammunition firing area. (LANL, 2007) This introduces a potential source of hot particles in dusts and other archived particulate matter, which may remain in the environment. LANL Airborne radionuclide surveillance has historically found higher uranium levels during windy periods, and saw elevated air uranium levels associated with the Cerro Grande fire. (Ibid, p. 108) Dust samples were sieved to pass a 150 micron screen and analyzed by gamma spectroscopy. Samples with higher activity were analyzed by Scanning Electron Microscopy/Energy Dispersive X-ray analysis, SEM/EDS. The results of gamma spectroscopy and individual particle counts were compared to determine the degree of radioactive heterogeneity in each sample. Radioactive heterogeneity, isotopic distribution, and particle size can be related to the source of the radioactive PM. Radiological contaminants in particulate matter, (PM), may exist as trace contamination in homogenous collections of particles, but may also exist heterogeneously, as a small number of high-concentration radionuclides among a larger set of uncontaminated particles. Residential and source area dusts were collected from locations surrounding, and potentially impacted, by operational and remedial activities at the HNR. The dust samples were analyzed, by multiple means, in order to identify those with radiologically- contaminated particles. Samples with higher activity were further analyzed by Scanning Electron Microscopy/Energy Dispersive X-ray analysis, (SEM/EDS), to determine if the radiological contamination was homogenous or heterogeneous. Two case studies were followed. The method isolated and analyzed lead and bismuth from naturally occurring radioactive material in coal fly ash. The method isolated and fingerprinted thorium, and the rare earths cerium, lanthanum, samarium, neodymium, and gadolinium in sedimentary cerium monazite minerals, nuclear waste processing dusts, and fission waste products in a WWTP effluent channel.

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