Methods and systems for detection of radionuclides

Disclosed are materials and systems useful in determining the existence of radionuclides in an aqueous sample. The materials provide the dual function of both extraction and scintillation to the systems. The systems can be both portable and simple to use, and as such can beneficially be utilized to determine presence and optionally concentration of radionuclide contamination in an aqueous sample at any desired location and according to a relatively simple process without the necessity of complicated sample handling techniques. The disclosed systems include a one-step process, providing simultaneous extraction and detection capability, and a two-step process, providing a first extraction step that can be carried out in a remote field location, followed by a second detection step that can be carried out in a different location

Simultaneous nitrate and oxygen respiration in coastal sediments: Evidence for discrete diagenesis

Oxygen and nitrate porewater profiles from sediments of Puget Sound, the Washington continental margin, and the Chukchi Sea were determined using a whole core squeezing apparatus. The two oxidants were observed to have equal sediment penetration depths and similar profile shapes in nearly all cores. Oxygen and nitrate, therefore, behaved in a similar manner in these shallow sediments: an observation that is not consistent with existing models of sediment diagenesis. A two-dimensional model was constructed in which nearly all oxidant (O2 and NO3−)consumption took place in scattered, highly reactive discrete micro-sites. The model produced a sedimentary environment in which reactions at each micro-site were limited by oxidant concentrations with oxidant gradients extending well beyond the micro-sites into relatively nonreactive bulk sediments. Thus for a given depth surface within the sediment, oxygen concentrations were much lower at micro-sites than average concentrations on that surface. Furthermore, at most micro-sites oxygen concentrations were sufficiently low enough to permit simultaneous denitrification, which explained the apparent similarity between oxygen and nitrate concentration profiles within these sediments. The model suggests that a relatively few, short-lived reaction sites are responsible for most oxygen and nitrogen reduction within oxic sediments under shallow seas, and it is consistent with emerging concepts about the fate of organic carbon in coastal sediments

Radioanalytical Chemistry for Automated Nuclear Waste Process Monitoring

Comparison of different pulse shape discrimination methods was performed under two different experimental conditions and the best method was identified. Beta/gamma discrimination of 90Sr/90Y and 137Cs was performed using a phoswich detector made of BC400 (2.5 cm OD x 1.2 cm) and BGO (2.5 cm O.D. x 2.5 cm ) scintillators. Alpha/gamma discrimination of 210Po and 137Cs was performed using a CsI:Tl (2.8 x 1.4 x 1.4 cm3) scintillation crystal. The pulse waveforms were digitized with a DGF-4c (X-Ray Instrumentation Associates) and analyzed offline with IGOR Pro software (Wavemetrics, Inc.). The four pulse shape discrimination methods that were compared include: rise time discrimination, digital constant fraction discrimination, charge ratio, and constant time discrimination (CTD) methods. The CTD method is the ratio of the pulse height at a particular time after the beginning of the pulse to the time at the maximum pulse height. The charge comparison method resulted in a Figure of Merit (FoM) of 3.3 (9.9 % spillover) and 3.7 (0.033 % spillover) for the phoswich and the CsI:Tl scintillator setups, respectively. The CTD method resulted in a FoM of 3.9 (9.2 % spillover) and 3.2 (0.25 % spillover), respectively. Inverting the pulse shape data typically resulted in a significantly higher FoM than conventional methods, but there was no reduction in % spillover values. This outcome illustrates that the FoM may not be a good scheme for the quantification of a system to perform pulse shape discrimination. Comparison of several pulse shape discrimination (PSD) methods was performed as a means to compare traditional analog and digital PSD methods on the same scintillation pulses. The X-ray Instrumentation Associates DGF-4C (40 Msps, 14-bit) was used to digitize waveforms from a CsI:Tl crystal and BC400/BGO phoswich detector

Colorimetric detection of uranium in water

Disclosed are methods, materials and systems that can be used to determine qualitatively or quantitatively the level of uranium contamination in water samples. Beneficially, disclosed systems are relatively simple and cost-effective. For example, disclosed systems can be utilized by consumers having little or no training in chemical analysis techniques. Methods generally include a concentration step and a complexation step. Uranium concentration can be carried out according to an extraction chromatographic process and complexation can chemically bind uranium with a detectable substance such that the formed substance is visually detectable. Methods can detect uranium contamination down to levels even below the MCL as established by the EPA

Polymer Sensors for the Quantification of Waterborne Uranium

Clandestine activities involving the separation, concentration or manipulation of special nuclear material for the express purpose of developing a weapon of mass destruction is likely to result in the contamination of environmental water sources. The capability to conduct isotopic analyses for waterborne special nuclear material, like uranium, would be a powerful nuclear forensics tool. Despite widespread interest, there currently is no on-line or field-able measurement system available for low-level quantification of uranium in aqueous solutions. A recent development in environmental sensing is a portable, flow cell detector that utilizes extractive scintillating (ES) resin. The ES resin serves the dual purpose of (1) concentrating the radionuclide of interest and (2) serving as a radiation transducer. Currently, such resins are produced by physically absorbing organic extractants and fluors into a polymer matrix. Unfortunately, this approach yields resins with poor stability as the active components leach from the resin over time. This contribution describes our work to increase resin stability by synthesizing ES resin in which the active components are bound covalently within the polymer matrix. The extraction and fluorescence properties of the resin were studied separately before the resin was applied in flow cell detector where detection efficiencies of 40% were achieved

Denitrification rates and excess nitrogen gas concentrations in the Arabian Sea oxygen deficient zone

Rates of canonical, i.e. heterotrophic, water-column denitrification were measured by 15N incubation techniques at a number of coastal and open ocean stations in the Arabian Sea. Measurements of N2:Ar gas ratios were also made to obtain independent estimates of N2 excess resulting from denitrification. Measured denitrification rates (15NO3-→15-14N2) at open ocean stations averaged 9.1±1.0 nmol N l-1 d-1 (n=15), and coastal rates averaged 33.2±12.4 nmol N l-1 d-1 (n=18). When extrapolated to the entire Arabian Sea, deep measurements within the offshore perennial suboxic zone indicate an overall denitrification rate of 41 Tg N a-1±18 Tg N a-1, which is within the range (10-44 Tg N a-1) of previous estimates for canonical denitrification in the region based on stoichiometric calculations and electron transport system activity. Nitrogen excess gas measurements predict a larger nitrogen anomaly than estimated by classical stoichiometric methods (maximum anomaly=23 μg at N l-1 vs. 13 μg at N l-1, respectively). This mismatch may result from incorrect assumptions of Redfield stoichiometry inherent in the nitrate deficit calculation, inputs of new nitrogen through N-fixation, N2 contributions from sedimentary denitrification along continental margins, the anammox reaction, and metal catalyzed denitrification reactions. Nevertheless, if denitrification is defined as the conversion of combined nitrogen to a gaseous end product, then the data suggest that denitrification in the Arabian Sea may have been underestimated so far

Radionuclide Sensors for Water Monitoring

Radionuclide contamination in the soil and groundwater at U.S. Department of Energy (DOE) sites is a severe problem that requires monitoring and remediation. Radionuclide measurement techniques are needed to monitor surface waters, groundwater, and process waters. Typically, water samples are collected and transported to an analytical laboratory, where costly radiochemical analyses are performed. To date, there has been very little development of selective radionuclide sensors for alpha- and beta-emitting radionuclides such as 90Sr, 99Tc, and various actinides of interest. The objective of this project is to investigate novel sensor concepts and materials for sensitive and selective determination of beta- and alpha-emitting radionuclide contaminants in water. To meet the requirements for low-level, isotope-specific detection, the proposed sensors are based on radiometric detection. As a means to address the fundamental challenge of the short ranges of beta and alpha particle s in water, our overall approach is based on localization of preconcentration/separation chemistries directly on or within the active area of a radioactivity detector. Automated microfluidics is used for sample manipulation and sensor regeneration or renewal. The outcome of these investigations will be the knowledge necessary to choose appropriate chemistries for selective preconcentration of radionuclides from environmental samples, new materials that combine chemical selectivity with scintillating properties, new materials that add chemical selectivity to solid-state diode detectors, new preconcentrating column sensors, and improved instrumentation and signal processing for selective radionuclide sensors. New knowledge will provide the basis for designing effective probes and instrumentation for field and in situ measurements

Radioanalytical Chemistry for Automated Nuclear Waste Process Monitoring

This research program is directed toward rapid, sensitive, and selective determination of beta and alpha-emitting radionuclides such as 99Tc, 90Sr, and trans-uranium (TRU) elements in low activity waste (LAW) processing streams. The overall technical approach is based on automated radiochemical measurement principles. Nuclear waste process streams are particularly challenging for rapid analytical methods due to the complex, high- ionic-strength, caustic brine sample matrix, the presence of interfering radionuclides, and the variable and uncertain speciation of the radionuclides of interest. As a result, matrix modification, speciation control, and separation chemistries are required for use in automated process analyzers. Significant knowledge gaps exist relative to the design of chemistries for such analyzers so that radionuclides can be quantitatively and rapidly separated and analyzed in solutions derived from low-activity waste processing operations. This research is addressing these knowledge gaps in the area of separation science, nuclear detection, and analytical chemistry and instrumentation. The outcome of these investigations will be the knowledge necessary to choose appropriate chemistries for sample matrix modification and analyte speciation control and chemistries for rapid and selective separation and preconcentration of target radionuclides from complex sample matrices. In addition, new approaches for quantification of alpha emitters in solution using solid state diode detectors, as well as improved instrumentation and signal processing techniques for use with solid-state and scintillation detectors, will be developed. New knowledge of the performance of separation materials, matrix modification and speciation control chemistries, instrument configurations, and quantitative analytical approaches will provide the basis for designing effective instrumentation for radioanalytical process monitoring. Specific analytical targets include 99 Tc, 90Sr and TRU actinides

Extraction-scintillation medium and method of use

An extraction-scintillation medium of substantially free-flowing, porous, solid particulate matter having one or more fluors retained within the particulate matter and an extraction agent adsorbed on or bound to the surface of the particulate matter. The medium is capable of extracting one of a selected radionuclide from an aqueous stream and permits transmission of light therethrough, which light is emitted from the one or more fluors in response to radiation absorbed thereby from the selected radionuclide. A sensor system using the extraction-scintillation medium for real-time or near real-time detection of the selected radionuclide is also disclosed