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[en] The Savannah River Site (SRS) Burial Ground had a container labeled as Box 33 for which they had no reliable solid waste stream designation. The container consisted of an outer box of dimensions 48-inch x 46-inch x 66-inch and an inner box that contained high density and high radiation dose material. From the outer box Radiation Control measured an extremity dose rate of 22 mrem/h. With the lid removed from the outer box, the maximum dose rate measured from the inner box was 100 mrem/h extremity and 80 mrem/h whole body. From the outer box the material was sufficiently high in density that the Solid Waste Management operators were unable to obtain a Co-60 radiograph of the contents. Solid Waste Management requested that the Analytical Development Section of Savannah River National Laboratory perform a γ-ray assay of the item to evaluate the radioactive content and possibly to designate a solid waste stream. This paper contains the results of three models used to analyze the measured γ-ray data acquired in an unusual configuration
[en] We have successfully incorporated high surface area particles of titanate ion exchange materials (monosodium titanate and crystalline silicotitanate) with acceptable particle size distribution into porous and inert support membrane fibrils consisting of polytetrafluoroethylene (Teflon(regsign)), polyethylene and cellulose materials. The resulting membrane sheets, under laboratory conditions, were used to evaluate the removal of surrogate radioactive materials for cesium-137 and strontium-90 from high caustic nuclear waste simulants. These membrane supports met the nominal requirement for nonchemical interaction with the embedded ion exchange materials and were porous enough to allow sufficient liquid flow. Some of this 47-mm size stamped out prototype titanium impregnated ion exchange membrane discs was found to remove more than 96% of dissolved cesium-133 and strontium-88 from a caustic nuclear waste salt simulants. Since in traditional ion exchange based column technology monosodium titanate (MST) is known to have great affinity for the sorbing of other actinides like plutonium, neptunium and even uranium, we expect that the MST-based membranes developed here, although not directly evaluated for uptake of these three actinides because of costs associated with working with actinides which do not have 'true' experimental surrogates, would also show significant affinity for these actinides in aqueous media. It was also observed that crystalline silicotitanate impregnated polytetrafluoroethylene or polyethylene membranes became less selective and sorbed both cesium and strontium from the caustic aqueous salt simulants
[en] A new rapid method for the determination of 226Ra in environmental samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used for emergency response or routine sample analyses. The need for rapid analyses in the event of a Radiological Dispersive Device or Improvised Nuclear Device event is well-known. In addition, the recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid analyses for radionuclides in environmental samples in the event of a nuclear accident. 226Ra (T1/2 = 1,620 years) is one of the most toxic of the long-lived alpha-emitters present in the environment due to its long life and its tendency to concentrate in bones, which increases the internal radiation dose of individuals. The new method to determine 226Ra in environmental samples utilizes a rapid sodium hydroxide fusion method for solid samples, calcium carbonate precipitation to preconcentrate Ra, and rapid column separation steps to remove interferences. The column separation process uses cation exchange resin to remove large amounts of calcium, Sr Resin to remove barium and Ln Resin as a final purification step to remove 225Ac and potential interferences. The purified 226Ra sample test sources are prepared using barium sulfate microprecipitation in the presence of isopropanol for counting by alpha spectrometry. The method showed good chemical recoveries and effective removal of interferences. The determination of 226Ra in environmental samples can be performed in less than 16 h for vegetation, concrete, brick, soil, and air filter samples with excellent quality for emergency or routine analyses. The sample preparation work takes less than 6 h. 225Ra (T1/2 = 14.9 day) tracer is used and the 225Ra progeny 217At is used to determine chemical yield via alpha spectrometry. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory radium particles are effectively digested. The preconcentration and column separation steps can also be applied to aqueous samples with good results.
[en] The Savannah River Site Environmental Bioassay Lab participated in the 2008 NRIP Emergency Response program administered by the National Institute for Standards and Technology (NIST) in May, 2008. A new rapid column separation method was used for analysis of actinides and 90Sr the NRIP 2008 emergency water and urine samples. Significant method improvements were applied to reduce analytical times. As a result, much faster analysis times were achieved, less than 3 hours for determination of 90Sr and 3-4 hours for actinides. This represents a 25%-33% improvement in analysis times from NRIP 2007 and a ∼100% improvement compared to NRIP 2006 report times. Column flow rates were increased by a factor of two, with no significant adverse impact on the method performance. Larger sample aliquots, shorter count times, faster cerium fluoride microprecipitation and streamlined calcium phosphate precipitation were also employed. Based on initial feedback from NIST, the SRS Environmental Bioassay Lab had the most rapid analysis times for actinides and 90Sr analyses for NRIP 2008 emergency urine samples. High levels of potential matrix interferences may be present in emergency samples and rugged methods are essential. Extremely high levels of 210Po were found to have an adverse effect on the uranium results for the NRIP-08 urine samples, while uranium results for NRIP-08 water samples were not affected. This problem, which was not observed for NRIP-06 or NRIP-07 urine samples, was resolved by using an enhanced 210Po removal step, which will be described.
[en] Characterization of transuranic waste is needed to make decisions about waste site remediation. Soil-gas sampling for xenon isotopes can be used to define the locations of spent fuel and transuranic wastes. Radioxenon in the subsurface is characteristic of transuranic waste and can be measured with extreme sensitivity using large-volume soil gas samples. Measurements at the Hanford Site showed 133Xe and 135Xe levels indicative of 240Pu spontaneous fission. Stable xenon isotopic ratios from fission are distinct from atmospheric xenon background. Neutron capture by 135Xe produces an excess of 136Xe in reactor-produced xenon providing a means of distinguishing spent fuel from separated transuranic materials
[en] Uranium-233 (t1/2 ∼ 1.59E5 years) is an artificial, fissile isotope of uranium that has significant importance in nuclear forensics. The isotope provides a unique signature in determining the origin and provenance of uranium-bearing materials and is valuable as a mass spectrometric tracer. Alpha spectrometry was employed in the critical evaluation of a 233U standard reference material (SRM-995) as a dual tracer system based on the in-growth of 229Th (t1/2 ∼ 7.34E3 years) for ∼35 years following radiochemical purification. Preliminary investigations focused on the isotopic analysis of standards and unmodified fractions of SRM-995; all samples were separated and purified using a multi-column anion-exchange scheme. The 229Th/233U atom ratio for SRM-995 was found to be 1.598E-4 (± 4.50%) using recovery-corrected radiochemical methods. Using the Bateman equations and relevant half-lives, this ratio reflects a material that was purified ∼ 36.8 years prior to this analysis. The calculated age is discussed in contrast with both the date of certification and the recorded date of last purification.
[en] A simple method for the electrodeposition of elemental arsenic (As) on a metal backing from aqueous solutions has been developed. The method was successfully applied to stable As (As-75). Thin (2.5 mg · cm-2) coherent, smooth layers of the metalloid on Ti foils (2.5 (micro)m thickness) were obtained. Electrodeposits served as targets for 75As(n,γ) 76As neutron capture experiments at Los Alamos Neutron Science Center (LANSCE). Respective 73As(n,γ) 74As experiments are planned for the near future, and 73As targets will be prepared in a similar fashion utilizing the introduced electrodeposition method. The preparation of an 73As (half-life 80.3 d) plating bath solution from proton irradiated germanium has been demonstrated. Germanium target irradiation was performed at the Los Alamos Isotope Production Facility (IPF)
[en] The Federal Bureau of Investigation (FBI) Laboratory is currently exploring needs and protocols for the storage of evidentiary items contaminated with radioactive material. While a large body of knowledge on the behavior of storage polymers in radiation fields exists, this knowledge has not been applied to the field of forensics and maintaining evidentiary integrity. The focus of this research was to evaluate the behavior of several traditional evidentiary containment polymers when exposed to significant alpha, beta, gamma, neutron and mixed radiation sources. Doses were designed to simulate exposures possible during storage of materials. Several products were found to be poorly suited for use in this specific application based on standardized mechanical testing results. Remaining products were determined to warrant further investigation for the storage of radiologically contaminated evidence.
[en] It is proposed to use 14 MeV neutrons tagged by the associated particle neutron time-of-flight technique (APnTOF) to identify the fillers of unexploded ordnances (UXO) by characterizing their carbon, nitrogen and oxygen contents. To facilitate the design and construction of a prototype system, a preliminary simulation model was developed, using the Geant4 toolkit. This work established the toolkit environment for (a) generating tagged neutrons, (b) their transport and interactions within a sample to induce emission and detection of characteristic gamma-rays, and (c) 2D and 3D-image reconstruction of the interrogated object using the neutron and gamma-ray time-of-flight information. Using the modeling, this article demonstrates the novelty of the tagged-neutron approach for extracting useful signals with high signal-to-background discrimination of an object-of-interest from that of its environment. Simulations indicated that an UXO filled with the RDX explosive, hexogen (C3H6O6N6), can be identified to a depth of 20 cm when buried in soil.
[en] The Savannah River Site Environmental Bioassay Lab participated in the 2007 NRIP Emergency Response program administered by the National Institute for Standards and Technology (NIST) in May, 2007. A new rapid column separation method was applied directly to the NRIP 2007 emergency urine samples, with only minimal sample preparation to reduce preparation time. Calcium phosphate precipitation, previously used to pre-concentrate actinides and Sr-90 in NRIP 2006 urine and water samples, was not used for the NRIP 2007 urine samples. Instead, the raw urine was acidified and passed directly through the stacked resin columns (TEVA+TRU+SR Resins) to separate the actinides and strontium from the NRIP urine samples more quickly. This improvement reduced sample preparation time for the NRIP 2007 emergency urine analyses significantly. This approach works well for small volume urine samples expected during an emergency response event. Based on initial feedback from NIST, the SRS Environmental Bioassay Lab had the most rapid analysis times for actinides and strontium-90 analyses for NRIP 2007 urine samples