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2016 Annual Inspection and Radiological Survey Results for the Piqua, Ohio, Decommissioned Reactor Site, July 2016

This report presents the findings of the annual inspection and radiological survey of the Piqua, Ohio, Decommissioned Reactor Site (site). The decommissioned nuclear power demonstration facility was inspected and surveyed on April 15, 2016. The site, located on the east bank of the Great Miami River in Piqua, Ohio, was in fair physical condition. There is no requirement for a follow-up inspection, partly because City of Piqua (City) personnel participated in a March 2016 meeting to address reoccurring safety concerns. Radiological survey results from 104 locations revealed no removable contamination. One direct beta activity reading in a floor drain on the 56-foot level (1674 disintegrations per minute [dpm]/100 square centimeters [cm2]) exceeded the minimum detectable activity (MDA). Beta activity has been detected in the past at this floor drain. The reading was well below the action level of 5000 dpm/100 cm2.

2016 Piqua↗

Design Study of an Incinerator Ash Conveyor Counting System - 13323

A design study has been performed for a system that should measure the Cs-137 activity in ash from an incinerator. Radioactive ash, expected to consist of both Cs-134 and Cs-137, will be transported on a conveyor belt at 0.1 m/s. The objective of the counting system is to determine the Cs-137 activity and direct the ash to the correct stream after a diverter. The decision levels are ranging from 8000 to 400000 Bq/kg and the decision error should be as low as possible. The decision error depends on the total measurement uncertainty which depends on the counting statistics and the uncertainty in the efficiency of the geometry. For the low activity decision it is necessary to know the efficiency to be able to determine if the signal from the Cs-137 is above the minimum detectable activity and that it generates enough counts to reach the desired precision. For the higher activity decision the uncertainty of the efficiency needs to be understood to minimize decision errors. The total efficiency of the detector is needed to be able to determine if the detector will be able operate at the count rate at the highest expected activity. The design study that is presented in this paper describes how the objectives of the monitoring systems were obtained, the choice of detector was made and how ISOCS (In Situ Object Counting System) mathematical modeling was used to calculate the efficiency. The ISOCS uncertainty estimator (IUE) was used to determine which parameters of the ash was important to know accurately in order to minimize the uncertainty of the efficiency. The examined parameters include the height of the ash on the conveyor belt, the matrix composition and density and relative efficiency of the detector. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Testing and Performance Validation of a Shielded Waste Segregation and Clearance Monitor Designed for the Measurement of Low Level Waste-13043

This paper describes the development, testing and validation of a shielded waste segregation and clearance monitor designed for the measurement of low-density low-level waste (LLW). The monitor is made of a measurement chamber surrounded by detectors and a shielded outer frame. The shielded chamber consists of a steel frame, which contains typically 1.5 inches (3.81 cm) of lead and 0.5 inches (1.27 cm) of steel shielding. Inside the shielding are plastic scintillator panels, which serve as gross gamma ray detectors. The detector panels, with embedded photomultipliers, completely surround the internal measurement chamber on all 6 sides. Care has been taken to distribute the plastic scintillator detectors in order to optimise both the efficiency for gamma ray detection and at the same time achieve a volumetric sensitivity, which is as uniform as possible. A common high voltage power supply provides the bias voltage for each of the six photomultipliers. The voltage signals arising from the detectors and photomultipliers are amplified by six sensitive amplifiers. Each amplifier incorporates a single channel analyser with both upper and lower thresholds and the digitised counts from each detector are recorded on six scalars. Operation of the device is by means of a microprocessor from which the scalars are controlled. An internal load cell linked to the microprocessor determines the weight of the waste object, and this information is used to calculate the specific activity of the waste. The monitor makes background measurements when the shielded door is closed and a sample, usually a bag of low-density waste, is not present in the measurement chamber. Measurements of the minimum detectable activity (MDA) of an earlier large volume prototype instrument are reported as part of the development of the Waste Segregation and Clearance Monitor (WSCM) described in the paper. For the optimised WSCM a detection efficiency of greater than 32% was measured using a small Cs-137 source placed in the centre of the measurement chamber. Small sources have also been used to determine the spatial variation of the detection efficiency for various positions within the measurement chamber. The data have been used to establish sentencing limits and different 'fingerprints' for specific waste streams including waste streams containing fission products and others based on other radionuclides including Am-241. Some of the test data that are presented have been used to validate the instrument performance. The monitor is currently in routine use at a nuclear facility for the measurement and sentencing of low-density low activity radioactive waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Investigation of Coincidence Counting for Improving Minimal Detectable Activity of 110m Ag in Single Particle Gamma Analysis

Post-irradiation examination (PIE) of fuel particles from the fourth Advanced Gas Reactor Fuel Development and Qualification (AGR) Program irradiation (AGR-5/6/7) is being performed at Oak Ridge National Laboratory (ORNL). Tristructural isotropic (TRISO)-coated particles and associated compacts for the AGR-5/6/7 experiment fabricated by BWX Technologies Nuclear Operations Group were formed into a graphite matrix compact and irradiated at the Advanced Test Reactor at Idaho National Laboratory. At ORNL, particles are deconsolidated from the graphite matrix compact and individually scanned for emitted gamma rays with the Irradiated Microsphere Gamma Analyzer (IMGA). The IMGA system comprises a single high purity germanium (HPGe) detector, an automated particle handling vacuum system, and an ORTEC DSPEC-50 digital spectrometer for gamma ray analysis. IMGA quantifies gamma ray-emitting fission product inventories of individual TRISO particles, and these inventories can be compared with the measured average inventories per particle and radionuclide inventories predicted by AGR-5/6/7 physics calculations to determine if a particle experienced radionuclide release. Details on IMGA data collection methods can be found in the literature. The TRISO particle’s SiC layer provides structural support, as well as a barrier for fission product release during irradiation or subsequent safety testing. A weakened or compromised SiC layer can be identified by the release of radionuclides, such as 137 Cs, which is detected by IMGA. However, select radionuclides, such as 90 Sr, 110 mAg, and 154 Eu have been shown to migrate through an intact SiC layer. Measurement of the radionuclide 110 mAg is significant as its release has been shown to be particularly sensitive to in-reactor conditions (e.g., temperature) with broad variable particle to-particle release behaviors observed within a single compact. As such, 110 mAg activity is often used for particle selection for comprehensive PIE as bounding 110 mAg retention particles are hypothesized to represent limits in particle behaviors within a compact. As TRISO particle fuel PIE activities continue over time, IMGA measurements of the 110 mAg inventory are eventually hindered because of its relatively short half-life (~250 days). As the fuel ages from its end of irradiation (EOI) date, the measurement uncertainty and minimum detectable activity (MDA) of 110m Ag increase because the detector background continuum begins to dominate. For particles from the second AGR irradiation experiment (AGR-2), the 110m Ag MDA was above 20% of the calculated average particle inventory after approximately five half-lives, and 110m Ag activity was no longer measurable with IMGA after approximately seven half-lives. Therefore, coincidence counting approaches have been explored to determine feasibility of leveraging new approaches to overcome limitations associated with increasing MDA over time.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design and Characterization of an Extremely-Sensitive, Large-Volume Gamma-Ray Spectrometer for Environmental Samples

A large volume gamma spectrometer was designed and constructed to analyze foodstuffs and environmental samples having low radionuclide concentrations. This system uses eight 11-cm × 42.5-cm × 5.5-cm NaI(Tl) detectors, chosen due to their relatively high sensitivity and availability and arranged in an octagonal configuration. The sensitive volume of the system is ~28 cm in diameter and ~42 cm deep. Shielding consists of an 86-cm × 86-cm square, 64-cm-tall lead brick enclosure with 18-cm-thick lead walls lined by 0.3-cm-thick copper plates. An aluminum top was machined to suspend the detectors within this shield. The shielding reduces background counts by 72% at 100 keV and 42% at 1,000 keV. The positional variability in sensitivity of the well was determined by both simulation and experiment. A 2.1-L volume of nearly uniform sensitivity, varying less than 10%, exists in the well's center. Energy resolutions of 14.6% and 7.8% were measured for 241 Am and 137 Cs, respectively. Energy resolution shows a 0.2% variation for both 241 Am and 137 Cs as a function of position within all regions of the well’s central sensitive volume. Dead time was also determined to be less than 35% for all sources measured in the system, the largest of which had an activity of 1,760 kBq. Simulated results for various source geometries show higher counts for smaller samples, especially at lower energies due to less attenuation of low energy photons. In conclusion, minimum detectable activities were determined for all source energies used, less than 5.1 Bq kg -1 for reasonable background and sample counting times.

47 OTHER INSTRUMENTATION↗

Comparison of two HPGe counting system used in activation studies for nuclear astrophysics

The activation method is a widely used technique to measure charged-particle induced cross sections for astrophys-ical applications. This two step technique is used for example to measure alpha-induced cross sections in γ-process related studies. The first step – in which a target is irradiated with a proton/alpha beam – is followed by the determination of the produced activity. Especially in p-process related studies in the heavier mass range, the produced radioactive nuclei decays mainly with electron-capture, resulting intense x-rays. The activity of the reaction products hence can be determine via the counting of these x-rays, and not only by counting the usually much weaker γ-rays. In this paper we compare the minimum detectable activity (MDA) of two High Purity Germanium (HPGe) detectors used for x- and γ-ray counting in activation experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurements of thorium and uranium daughters in radioenvironmental samples using γ γ -coincidence spectrometry

We present the performance of a γ γ -coincidence spectrometer for measuring the activities of thorium and uranium daughters in environmental samples. The spectrometer consists of two NaI(Tl) detectors facing each other inside a low-background passive shield. We present coincidence gating schemes for achieving the best signal-to-noise ratios, coincidence detection efficiencies, background levels, and minimum detectable activities. The spectrometer is simulated using Geant4 to correct sample efficiencies for self-absorption effects. The device is used to measure thorium and uranium daughter activities in Brazil nuts, potting mix, and magazine paper. Our results for Brazil nuts agree with some, but not all, previous measurements. Thorium or uranium daughter activities have previously not been reported for commercial potting mix. For magazine paper, our measured activities are lower than most previously determined values.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Liquid scintillation counting methodology for 99 Tc analysis. A remedy for radiopharmaceutical waste

This paper presents a new approach for liquid scintillation counting (LSC) analysis of single-radionuclide samples containing appreciable organic or inorganic quench. This work offers better analytical results than existing LSC methods for technetium-99 ( 99g Tc) analysis with significant savings in analysis cost and time. The method was developed to quantify 99g Tc in environmental liquid and urine samples using LSC. Method efficiency was measured in the presence of 1.9 to 11,900 ppm total dissolved solids. The quench curve was proved to be effective in the case of spiked 99g Tc activity calculation for deionized water, tap water, groundwater, seawater, and urine samples. Counting efficiency was found to be 91.66% for Ultima Gold LLT (ULG-LLT) and Ultima Gold (ULG). Relative error in spiked 99g Tc samples was ±3.98% in ULG and ULG-LLT cocktails. Minimum detectable activity was determined to be 25.3 mBq and 22.7 mBq for ULG-LLT and ULG cocktails, respectively. A pre-concentration factor of 1000 was achieved at 100°C for 100% chemical recovery.

Cocktail↗

Performance Assessment of a New Gamma Spectroscopy Toolkit: Peak Doctor and the Spectral Nondestructive Assay Platform (SNAP) - 17397

High resolution gamma spectroscopy (HRGS) is a widely used technique for non-destructive characterization of nuclear materials, and assay of radioactive waste. The ability to accurately evaluate raw spectral data is an important step in producing high-quality results. A spectral analysis application known as Peak Doctor has been developed under a Cooperative Research and Development Agreement (CRADA) between LANL and Pajarito Scientific Corporation (PSC). The software has undergone several years of testing and validation by the Radioactive Waste Characterization Team of the LANL Waste Management Services Group (WM-SVS). PeakDoctor is designed to work with the Spectral Nondestructive Assay Platform (SNAP{sup TM}) to provide a complete HRGS analysis engine. SNAP{sup TM} performs model specific corrections for attenuation and geometry. These applications are the major components of a new toolkit designed primarily for portable far-field non-destructive assay. Peak Doctor performs a very accurate peak fit analysis with the goal of improving upon the capabilities of existing commercially available routines. It is designed to be user-configurable and can be customized to any given type of detector and any given type of spectrum. Peak Doctor was developed to resolve many of the inherent complexities in gamma ray spectra including overlapping peaks, complex multiplet regions, large step peaks, backscatter regions and Compton edges. Unlike most spectral analysis platforms, Peak Doctor does not rely on the energy calibration and detector resolution parameters that are saved by the operator in the spectrum file. Instead, key parameters are pre-defined for individual detectors. The software fits a continuum using a series of splines between a series of junctions or 'knots'. Fitting techniques are used to join the splines together to create a near-continuous multi-element curve. Optimizing the location of the knots is one of Peak Doctor's most powerful features. The knots are initially configured using a pre-defined list and are removed or added automatically during the fitting process. Knots are also created when new features are identified such as Step Peaks and Compton Edges. The user can also manually specify knots in order to improve the continuum fit. The initial fit is improved on by removing any outlier regions (which are converted to peaks) and the continuum fitting process is repeated. At this stage, an experienced user can work interactively with the fit by manually converting peak regions to continuum or vice versa. The final step is to fit a series of peaks above the continuum based on detector parameters. Single and multiplet peaks are then processed by either the tailing (piecewise) or non-tailing (Gaussian) Levenberg Marquardt non-linear peak fitting routine depending on the user defined selection. Only a rough knowledge of the detector characteristics (energy calibration and resolution) is required for the fitting process to proceed with good accuracy. Any peaks that are missed can be manually added by the user and will also be fitted. Discontinuities in the peak / continuum fit can be rapidly identified by reviewing the 'residuals scale' plot. For waste streams that are well characterized, it is often the case that routinely encountered spectra will have similar peaks and continuum features. For these cases a handy 'One Step' method is available that proceeds in an automated fashion without user interaction. Peak Doctor has been configured with a set of default spectrum types including plutonium / transuranic waste (including Weapons Grade Pu, Heat Source Pu, Am-241, Am-243 and Np-237), depleted or enriched uranium, nuclear power plant / intermediate level waste (with fission and activation products such as Cs-137 and Co-60) as well as Naturally Occurring Radioactive Materials (NORM). The user can easily add new spectrum types for specific waste streams or other types of radiological / special nuclear materials. The output from PeakDoctor (including net peak area, centroid energy and a list of minimum detectable activity levels at pre-defined regions) is used by SNAP{sup TM} to complete the data analysis process. Isotope activities are calculated using configurable template-driven geometry and attenuation correction methods. The software accounts for matrix and container wall effects, collimator / angular corrections, detector efficiency (based on calibration curves) and stand-off distance. SNAP{sup TM} uses published algorithms incorporating a series of decision points during its operation to allow the analyst to provide logical input to guide the software during the analysis of each unique spectrum. The Peak Doctor / SNAP{sup TM} toolkit has been extensively tested and validated under a variety of conditions using 'benchmark' reference spectra. Test scenarios reported include HPGe-based measurements of well characterized uranium and plutonium standards and radioactive sources with a variety of different geometries and matrix materials including surrogate drums and boxes. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Rapid determination of radiostrontium in seawater samples

A new method for the determination of radiostrontium in seawater samples has been developed at the Savannah River National Laboratory (SRNL) that allows rapid preconcentration and separation of strontium and yttrium isotopes in seawater samples for measurement. The new SRNL method employs a novel and effective pre-concentration step that utilizes a blend of calcium phosphate with iron hydroxide to collect both strontium and yttrium rapidly from the seawater matrix with enhanced chemical yields. The pre-concentration steps, in combination with rapid Sr Resin and DGA Resin cartridge separation options using vacuum box technology, allow seawater samples up to 10 liters to be analyzed. The total 89 Sr + 90 Sr activity may be determined by gas flow proportional counting and recounted after ingrowth of 90 Y to differentiate 89 Sr from 90 Sr. Gas flow proportional counting provides a lower method detection limit than liquid scintillation or Cerenkov counting and allows simultaneous counting of samples. Simultaneous counting allows for longer count times and lower method detection limits without handling very large aliquots of seawater. Seawater samples up to 6 liters may be analyzed using Sr Resin for 89 Sr and 90 Sr with a Minimum Detectable Activity (MDA) of 1-10 mBq/L, depending on count times. Seawater samples up to 10 liters may be analyzed for 90 Sr using a DGA Resin method via collection and purification of 90 Y only. If 89 Sr and other fission products are present, then 91 Y (beta energy 1.55 MeV, 58.5 day half-life) is also likely to be present. 91 Y interferes with attempts to collect 90 Y directly from the seawater sample without initial purification of Sr isotopes first and 90 Y ingrowth. The DGA Resin option can be used to determine 90 Sr, and if 91 Y is also present, an ingrowth option with using DGA Resin again to collect 90 Y can be performed. An MDA for 90 Sr of <1 mBq/L for an 8 hour count may be obtained using 10 liter seawater sample aliquots.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A Single Tower Configuration of the Modular Gamma Box Counter System - 13392

Canberra's Standard Gamma Box Counter System is designed to perform accurate quantitative assays of gamma emitting nuclides for a wide range of large containers including B-25 crates and ISO shipping containers. Using a modular building-block approach, the system offers tremendous flexibility for a variety of measurement situations with wide ranges of sample activities and throughput requirements, as well as the opportunity to modify the configuration for other applications at a later date. The typical configuration consists of two opposing towers each equipped with two high purity germanium detectors, and an automated container trolley. This paper presents a modified configuration, consisting of a single tower placed inside a measurement trailer with three detector assemblies, allowing for additional vertical segmentation as well as a viewing a container outside the trailer through the trailer wall. An automatic liquid nitrogen fill system is supplied for each of the detectors. The use of a forklift to move the container for horizontal segmentation is accommodated by creating an additional operational and calibration set-up in the NDA 2000 software to allow for the operator to rotate the container and assay the opposite side, achieving the same sensitivity as a comparable two-tower system. This Segmented Gamma Box Counter System retains the core technologies and design features of the standard configuration. The detector assemblies are shielded to minimize interference from environmental and plant background, and are collimated to provide segmentation of the container. The assembly positions can also be modified in height and distance from the container. The ISOCS calibration software provides for a flexible approach to providing the calibrations for a variety of measurement geometries. The NDA 2000 software provides seamless operation with the current configuration, handling the data acquisition and analysis. In this paper, an overview of this system is discussed, along with the measured performance results, calibration methodology and verification, and minimum detectable activity levels. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Type A Verification Report for the High Flux Beam Reactor Stack and Grounds, Brookhaven National Laboratory, Upton, New York

The U.S. Department of Energy (DOE) Order 458.1 requires independent verification (IV) of DOE cleanup projects (DOE 2011). The Oak Ridge Institute for Science and Education (ORISE) has been designated as the responsible organization for IV of the High Flux Beam Reactor (HFBR) Stack and Grounds area at Brookhaven National Laboratory (BNL) in Upton, New York. The IV evaluation may consist of an in-process inspection with document and data reviews (Type A Verification) or a confirmatory survey of the site (Type B Verification). DOE and ORISE determined that a Type A verification of the documents and data for the HFBR Stack and Grounds: Survey Units (SU) 6, 7, and 8 was appropriate based on the initial survey unit classification, the walkover surveys, and the final analytical results provided by the Brookhaven Science Associates (BSA). The HFBR Stack and Grounds surveys began in June 2011 and were completed in September 2011. Survey activities by BSA included gamma walkover scans and sampling of the as-left soils in accordance with the BSA Work Procedure (BNL 2010a). The Field Sampling Plan - Stack and Remaining HFBR Outside Areas (FSP) stated that gamma walk-over surveys would be conducted with a bare sodium iodide (NaI) detector, and a collimated detector would be used to check areas with elevated count rates to locate the source of the high readings (BNL 2010b). BSA used the Mult- Agency Radiation Survey and Site Investigation Manual (MARSSIM) principles for determining the classifications of each survey unit. Therefore, SUs 6 and 7 were identified as Class 1 and SU 8 was deemed Class 2 (BNL 2010b). Gamma walkover surveys of SUs 6, 7, and 8 were completed using a 2X2 NaI detector coupled to a data-logger with a global positioning system (GPS). The 100% scan surveys conducted prior to the final status survey (FSS) sampling identified two general soil areas and two isolated soil locations with elevated radioactivity. The general areas of elevated activity identified were investigated further with a collimated NaI detector. The uncollimated average gamma count rate was less than 15,000 counts per minute (cpm) for the SU 6, 7, and 8 composite area (BNL 2011a). Elevated count rates were observed in portions of each survey unit. The general areas of elevated counts near the Building 801 ventilation and operations and the entry to the Stack were determined to be directly related to the radioactive processes in those structures. To compensate for this radioactive shine, a collimated or shielded detector was used to lower the background count rate (BNL 2011b and c). This allowed the surveyor(s) to distinguish between background and actual radioactive contamination. Collimated gamma survey count rates in these shine affected areas were below 9,000 cpm (BNL 2011a). The average background count rate of 7,500 cpm was reported by BSA for uncollimated NaI detectors (BNL 2011d). The average collimated background ranged from 4,500-6,500 cpm in the westernmost part of SU 8 and from 2,000-3,500 cpm in all other areas (BNL 2011e). Based on these data, no further investigations were necessary for these general areas. SU 8 was the only survey unit that exhibited verified elevated radioactivity levels. The first of two isolated locations of elevated radioactivity had an uncollimated direct measurement of 50,000 cpm with an area background of 7,500 cpm (BNL 2011f). The second small area exhibiting elevated radiation levels was identified at a depth of 6 inches from the surface. The maximum reported count rate of 28,000 cpm was observed during scanning (BNL 2011g). The affected areas were remediated, and the contaminated soils were placed in an intermodal container for disposal. BSA&#x27;s post-remediation walkover surveys were expanded to include a 10-foot radius around the excavated locations, and it was determined that further investigation was not required for these areas (BNL 2011 f and g). The post-remediation soil samples were collected and analyzed with onsite gamma spectroscopy equipment. These samples were also included with the FSS samples that were analyzed at an offsite facility for the primary radionuclides of concern (ROCs) (i.e., cesium-137, strontium-90, and radium-226). Analysis included full spectrum gamma spectroscopy for all samples. Sr-90 analysis was completed on all samples from SUs 6 and 7. However Sr-90 was only completed on the cores, composites, field blank and duplicate samples in SU 8. Alpha spectroscopy as well as liquid scintillation performed for tritium, carbon-14, and nickel-63 concentrations were completed on the composite samples from SUs 6 and 7. Various cores, composites, and samples from the remediated areas of SU 8 received alpha spectroscopy as well as liquid scintillation analyses for tritium, carbon-14, and nickel-63 to determine respective ROC concentrations (BNL 2011 h, i, and j). BSA submitted the FSS data and analytical results to demonstrate that remediation efforts complied with the specified cleanup goal of less than or equal to 15 millirem per year (mrem/yr) above background to a resident in 50 years (BNL 2011a through j). ORISE has reviewed the project documentation and FSS data for the HFBR Stack and Grounds: SUs 6, 7, and 8. The highest concentrations of the primary ROCs reported were 5.92 picocuries per gram (pCi/g) for Cs-137 and 2.03 pCi/g for Sr-90, with both ROCs having the qualifier for the sample result as less than the minimum detectable activity (MDA). For Ra-226, the highest detected concentration from the FSS data provided was 0.682 pCi/g. Other potential secondary contaminants were below their respective MDAs. Therefore, ORISE is of the opinion that BSA has provided sufficient evidence to demonstrate compliance with the 15 mrem/yr cleanup objectives for the final status survey data provided.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Liquid Scintillation Counting of Environmental Radioisotopes: A Review of the Impact of Background Reduction

Liquid scintillation counting (LSC) is a versatile and commonplace method for radiometric measurement of charged particle emitting radionuclides. The LSC method provides utility in a range of environmental science applications including hydrological studies of water transport, anthropogenic releases of radionuclides into the environment, and vertical mixing rates within oceans. Instrumental measurement background is one limiting factor of radiometric measurement sensitivity. As part of the development of a custom low background LSC system located in a shallow underground laboratory at Pacific Northwest National Laboratory, a number of measurement applications of LSC have been considered and are summarized here. The focus is on determining which aspects of such measurements would gain the greatest benefit from the reduction of LSC backgrounds by a factor of 10-100 relative to values reported in the literature. Examples of benefits include lowering the minimum detectable activity, reducing the sample size required, and shortening the elapsed timeline of the processing and analysis sequence. In particular tritium, strontium, and actinium isotopes are examined as these isotopes cover a range of requirements related to the LSC measurement method (e.g., 3H: low energy; Sr: spectral deconvolution; Ac: alpha/beta discrimination).

actinium↗

RAPID QUANTITATION OF URANIUM FROM MIXED FISSION PRODUCT SAMPLES

Chemical similarities between U(VI) and Mo(VI) create challenges for separation and quantification of uranium from a mixed fission product sample. The purpose of this work was to demonstrate the feasibility of using Eichrom’s® UTEVA resin in addition to a tellurium spontaneous deposition to improve the quantitation of 235U using gamma spectroscopy. The optimized method demonstrated a consistent chemical yield of 74 ± 3 % for uranium. This procedure was evaluated using 1.41x1012 fissions produced from an irradiated HEU sample. The uranium was isotopically yielded by HPGe, and the minimum detectable activity (MDA) determined from the gamma spectra. The MDA for 235U, 237U, and 238U was reduced by a factor of two. The chemical isolation of uranium was successfully achieved in less than four hours, with a separation factor of 1.41x105 from molybdenum.

Haney, Morgan M.↗

Rapid method to determine 89 Sr/ 90 Sr in large concrete samples

Here, a new rapid method has been developed that provides high quality low-level measurements of 89,90 Sr in concrete samples with an MDA (Minimum Detectable Activity) of <1 mBq g -1 . The new method is fast, meets new decommissioning regulatory limits and is robust even if refractory particles are present. The method utilizes a rapid fusion to ensure total dissolution of samples and rapid preconcentration and separation of 89,90 Sr from 5-10 g concrete samples. When, the 89 Sr/ 90 Sr ratio is high, Sr can be isolated from up to 5g concrete samples, total 89/90 Sr measured, and then 90Sr determined via 90 Y separated after a period of ingrowth. Another approach allows the immediate determination of 90 Sr in 10 g concrete aliquots without waiting for 90 Y ingrowth, in instances where the shorter lived 89 Sr is unlikely to be encountered.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Alpha/beta-gated gamma–gamma spectroscopy of mixed fission products for trace analysis

This experiment demonstrated that some hard-to-detect fission products can be quantified directly from mixed fission product samples using advanced radio-emission spectroscopy techniques. A gamma/gamma coincidence detector was combined with a custom liquid scintillation counter to evaluate the benefits of alpha and beta coincident and anti-coincident analysis of mixed fission product samples. Reduction factors in the minimum detectable activity (MDA) relative to traditional gamma counting were quantified for a set of radionuclides. For isotopes like 91Y, 144Ce, 147Nd, and 153Sm MDA reductions of factors of 1-2 were observed using optimized beta thresholds. Using beta anti-coincidence counting reductions of factors 3-5 were observed for isotopes like 89Sr, 95mNb, 115Cd, and 137Cs and factors of 5-7 for isotopes like 235U using alpha coincidence counting. The selectivity of gamma/gamma coincidence and reduction in backgrounds using beta gating were also demonstrated with 136Cs and 153Sm. The improvements observed in the detection sensitivity of fission products and actinides achieved by combining time-correlated radiation signatures is significant and of value to applications such as nuclear fission physics, environmental monitoring for nuclear waste, reactor accidental releases, and nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A low-background γγ-coincidence spectrometer for radioisotope studies

The performance of a new, low-background NaI(Tl) spectrometer, based on γγ-coincidence counting, is discussed. We present experimental coincidence efficiencies, timing resolutions, background count rates, and minimum detectable activities. The spectrometer has been simulated using Geant4, and the results are used for estimating coincidence efficiencies for volume sources. To test the device, we measured the cosmogenic 26 Al activity in a small (17.7 g) meteorite fragment. Here, we find a value of 52.9±7.8 dpm / kg, in agreement with the activity measured previously in a much larger fragment of the same meteorite using a HPGe detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗