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Radioactive decay of $\mathrm {{}^{90}Sr}$ in cement: a non-equilibrium first-principles investigation

Cement is an inexpensive and relatively easily manageable material that is used as a last barrier for nuclear waste disposal. Under these conditions, the cement is in contact with low radiation doses, but there is a distinct possibility of being contaminated with radioactive products. Of particular concern is the medium lived half-life product 90 Sr (28.8 years) due to its ability to replace Ca. 90 Sr undergoes β-decay to 90 Y which, in turn, β-decays to stable 90 Zr. In this work, we discuss systematically the chain of non-equilibrium processes that result as a consequence of β-decay events in cement. We first use density functional-based methods to study the consequences of the sudden increase of the nuclear charge from Z to Z+1, a possible induced ionization and the perturbation of the surrounding electronic charge. Secondly, we use molecular dynamics simulations to study the recoil of the daughter nucleus. Finally, we discuss the damage caused by the ionization cascade produced during the propagation of the β-electron and the resulting chemical and structural perturbation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radsource Mr: Mixed Reality Planning Tool For Radioactive Recovery

The RadSource MR system leverages Meta Quest 3's advanced mixed reality capabilities to create a comprehensive spatial planning platform for end-of-life sealed radioactive source recovery operations. The application utilizes the Quest 3's high-resolution passthrough cameras and spatial mapping algorithms to generate accurate 3D environmental models. Core technical components include: (1) Real-time spatial measurement algorithms calculating distances, angles, slopes, and surface areas with sub-centimeter accuracy; (2) Virtual object placement system allowing users to position digital representations of recovery equipment (trailers, containment vessels, protective barriers) within the real environment; (3) Voice recording and annotation system for hands-free documentation in protective equipment; (4) 3D mesh capture and storage capabilities for post-operation analysis and regulatory documentation. (5) Procedure documentation is available for viewing in Mixed Reality, providing an innovative and convenient way to access the information during pre-visit and inspection activities. (6) Support for screen capture for the view for real world and virtual objects together to use it later for planning. The system integrates computer vision techniques for environmental understanding, spatial mathematics for precise measurements, and human-computer interaction principles optimized for hazardous environment operations. Data persistence allows teams to save and share planning sessions across multiple stakeholders while maintaining operational security requirements.

Khadka, Rajiv [Idaho National Laboratory (INL), Id↗

Microfluidic-Based sample chips for radioactive solutions

Historical nuclear fuel cycle process sampling techniques required sample volumes ranging in the tens of milliliters. The radiation levels experienced by analytical personnel and equipment, in addition to the waste volumes generated from analysis of these samples, have been significant. These sample volumes also impacted accountability inventories of required analytes during process operations. To mitigate radiation dose and other issues associated with the historically larger sample volumes, a microcapillary sample chip was chosen for further investigation. The ability to obtain microliter volume samples coupled with a remote automated means of sample loading, tracking, and transporting to the analytical instrument would greatly improve analytical efficiency while reducing both personnel exposure and radioactive waste volumes. Sample chip testing was completed to determine the accuracy, repeatability, and issues associated with the use of microfluidic sample chips used to supply µL sample volumes of lanthanide analytes dissolved in nitric acid for introduction to an analytical instrument for elemental analysis.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effect of seawater intrusion on radioactive strontium (90Sr) sorption and transport at nuclear power plants

Batch sorption and column experiments were conducted to investigate and compare sorption and transport behavior of 90Sr on the assumption of seawater intrusion at nuclear power plants. Batch sorption experiments were carried out on fractured rocks and bedrocks using synthetic groundwater and seawater both spiked with 90Sr. In general, higher 90Sr sorption occurred on fractured rock samples than on bedrocks, because of the presence of weathered secondary minerals (iron oxide and clay) on fractured rock surfaces. However, one particular bedrock sample (WSP-B) which has higher porosity and carbon amount than fractured rock samples also showed the higher 90Sr sorption than its comparable fractured rocks. For all batch sorption studies, 90Sr sorption distribution coefficient, Kd decreased from groundwater to seawater environment due to the higher ionic strength of seawater (6.4×10-1–7.7×10-1 M) compared to groundwater (4.0×10-3–6.0×10-3 M). The three different ionic strength solutions were used in column experiments, and the results showed that transport behavior of Sr through a fractured rock had similar sorption trend to batch sorption results. The highest mobility (or least retardation) for Sr was found for 100% seawater solution compared to the highest retardation (or least mobility) for 100% groundwater solution. These sorption and transport data of Sr on solid materials contacted with various ionic strength solutions corroborate empirically defensible information for assessment of radioactive contamination in groundwater below the NPP sites located nearby shores. In addition, the experimental data will be incorporated to improve transport models of 90Sr in the subsurface environment for severe nuclear accidents.

Chang, Seeun↗

Performance of detectors used in measurements of radioactive materials deposited in tissues from intakes by wounds

In the care of people injured with wounds with incorporated radioactive material, the basic information is collected, using appropriate detectors, following procedures established in first aid protocol. The reliability of the data collected for medical treatment depends greatly on the metrological performance of the equipment, the experimental set up and the scenario of the occurrence of the accident. The methodology to evaluate the performance of the detectors use the comparison of the attenuation coefficient value of each radionuclide obtained by the attenuation curve of tissue-equivalent material to the theoretical value established by NIST in each experimental set up. The good performance was defined when the difference between the experimental and theoretical value is close to zero. The experimental set ups were chosen according to the types of possible measurements performed in the various scenarios of the radiological accident. The detectors used were Personal Radiation Dosimeter, IdentiFINDER2, Cadmium Telluride and Hyper Pure Germanium. Furthermore, the results for 241 Am showed better performance with HPGe and IdentiFINDER2 shielded. For the 60 Co the best performance occurred with the shielded and collimated IdentiFINDER2. For the 137 Cs, the HPGe detector presented the best performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Reduction in radioactivity-induced backgrounds using a novel active veto detector for rare event search experiments

The results of a newly developed annular cryogenic phonon-mediated active veto detector are discussed which shows a significant reduction of radioactivity-induced backgrounds in rare event search experiments. The veto detector is made up of germanium weighing ∼500 g with an outer diameter of 76 mm and an inner diameter of 28 mm. The detector can host a 25 mm diameter germanium inner target detector of mass ∼10 g. A GEANT4 simulation with the active veto and inner target detector shows a gamma background reduction of 50 - 80% which is further improved (> 90%) with 4pi veto coverage. Experimental measurements with the detector assembly agree well with the simulation.

Chaudhuri, Mouli↗

Nevada National Security Site 2010 Data Report: Groundwater Monitoring Program Area 5 Radioactive Waste Management Site

This report is a compilation of the groundwater sampling results from the Area 5 Radioactive Waste Management Site (RWMS). The data have been collected since 1993 and include calendar year 2010 results. During 2010, groundwater samples were collected and static water levels were measured at the three pilot wells surrounding the Area 5 RWMS. Samples were collected at UE5PW-1 on March 10 and August 10, 2010; at UE5PW-2 on March 10, August 10, and August 25, 2010; and at UE5PW-3 on March 31, August 10, and August 25, 2010. Static water levels were measured at each of the three pilot wells on March 1, April 26, August 9, and November 9, 2010. Groundwater samples were analyzed for the following indicators of contamination: pH, specific conductance, total organic carbon, total organic halides, and tritium. Indicators of general water chemistry (cations and anions) were also measured. Results from all samples collected in 2010 were within the limits established by agreement with the Nevada Division of Environmental Protection for each analyte. These data indicate that there has been no measurable impact to the uppermost aquifer from the Area 5 RWMS. There were no significant changes in measured groundwater parameters compared to previous years. The report contains an updated cumulative chronology for the Area 5 RWMS Groundwater Monitoring Program and a brief description of the site hydrogeology.

54 ENVIRONMENTAL SCIENCES↗

Small-angle Compton Scattering to Determine the Depth of a Radioactive Source in Matter

A gamma-ray peak in a spectrum is often accompanied by a discontinuity in the Compton continuum at the peak. The Compton continuum results from Compton scattering in the detector. The discontinuity at a peak results from small-angle Compton scattering by the gamma rays in matter situated directly between the gamma-ray source and the detector. The magnitude of this discontinuity with respect to the gamma-ray peak is therefore an indicator of the amount of material or shielding between the gamma-ray source and the detector. This small-angle scattering was used to determine the depth of highly-enriched uranium (HEU) solution standards in a concrete floor mockup. The empirical results of the use of this small-angle scattering discontinuity in a concrete floor experiment will be described. A Monte Carlo calculation of the experiment will also be described. In addition, the depth determined from small-angle scattering was used in conjunction with differential attenuation to more accurately measure the uranium content of the mockup. Following these empirical results, the theory of small-angle scattering will be discussed. The magnitude of the discontinuity compared to the peak count rate is directly related to the depth of the gamma-ray source in matter. This relation can be described by relatively simple mathematical expressions. This is the first instance that we are aware of in which the small-angle Compton scattering has been used to determine the depth of a radioactive source. Furthermore this is the first development of the theoretical expressions for the magnitude of the small-angle scattering discontinuity.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

RESULTS FROM ANALYSIS OF THE FIRST AND SECOND STRIP EFFLUENT COALESCER ELEMENTS FROM RADIOACTIVE OPERATIONS OF THE MODULAR CAUSTIC-SIDE SOLVENT EXTRACTION UNIT

The coalescer elements for the Strip Effluent (SE) acid within the Modular Caustic-Side Solvent Extraction Unit (MCU) experienced elevated differential pressure drop during radioactive operations. Following the end of operations for the first Macrobatch campaign and soon after start of the second Macrobatch campaign, personnel removed the coalescer media and provided to Savannah River National Laboratory (SRNL) for diagnostic investigation of the causes of reduced flow. This report summarizes those studies. Two Strip Effluent (SE) coalescers were delivered to the Savannah River National Laboratory (SRNL). One was removed from the Modular Caustic-Side Solvent Extraction Unit (MCU) between processing of Macrobatch 1 and 2 (coalescer 'Alpha'), and the second was removed from MCU after processing of {approx}24,000 gallons of salt solution (coalescer 'Beta'). Both coalescers underwent the same general strip acid flush program to reduce the dose and were delivered to SRNL for analysis of potential occluding solids. Analysis of Coalescer Alpha indicates the presence of aluminum hydroxide solids and aluminosilicate solids, while analysis of Coalescer Beta indicates the presence of aluminum hydroxide solids, but no aluminosilicates. Leaching studies on sections of both coalescers were performed. The results indicate that the coalescers had different amounts of solids present on them at the time of removal. Finally, samples of free liquids retrieved from both coalescers indicate no excessive amounts of CSSX solvent present. Given the strip acid flushing that occurred in the SE coalescers, the solids we detected on the coalescers are probably indicative of a larger quantity of these solids present before the strip acid flushing. Under this scenario, the excessive pressure drops are due to the solids and not from organic fouling.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Human machine interface (hmi) evaluation of rooms ta-50-1-60/60a at the radioactive liquid waste treatment facility (rlwtf)

This effort addressed an evaluation of human machine interfaces (HMIs) in Room TA-50-1-60/60A of the Radioactive Liquid Waste Treatment Facility (RLWTF). The evaluation was performed in accordance with guidance outlined in DOE-STD-3009, DOE Standard Preparation Guide for U.S. Department of Energy Nonreactor Nuclear Facility Documented Safety Analyses, 2006 [DOE 2006]. Specifically, Chapter 13 of DOE 2006 highlights the 10 CFR 830, Nuclear Safety Management, 2012, [CFR 2012] and DOE G 421.1-2 [DOE 2001a] requirements as they relate to the human factors process and, in this case, the safety of the RLWTF. The RLWTF is a Hazard Category 3 facility and, consequently, does not have safety-class (SSCs). However, safety-significant SSCs are identified. The transuranic (TRU) wastewater tanks and associated piping are the only safety-significant SSCs in Rooms TA-50-1-60/60A [LANL 2010]. Hence, the human factors evaluation described herein is only applicable to this particular assemblage of tanks and piping.

42 ENGINEERING↗

Radioactive Semivolatiles in Nuclear Fuel Reprocessing

In nuclear fuel reprocessing, various radioactive elements enter the gas phase from the unit operations found in the reprocessing facility. In previous reports, the pathways and required removal were discussed for four radionuclides known to be volatile, 14 C, 3 H, 129 I, and 85 Kr. Other, less volatile isotopes can also report to the off-gas streams in a reprocessing facility. These were reported to be isotopes of Cs, Cd, Ru, Sb, Tc, and Te. In this report, an effort is made to determine which, if any, of 24 semivolatile radionuclides could be released from a reprocessing plant and, if so, what would be the likely quantities released. As part of this study of semivolatile elements, the amount of each generated during fission is included as part of the assessment for the need to control their emission. Also included in this study is the assessment of the cooling time (time out of reactor) before the fuel is processed. This aspect is important for the short-lived isotopes shown in the list, especially for cooling times approaching 10 y. The approach taken in this study was to determine if semivolatile radionuclides need to be included in a list of gas-phase radionuclides that might need to be removed to meet Environmental Protection Agency (EPA) and Nuclear Regulatory Commission (NRC) regulations. A list of possible elements was developed through a literature search and through knowledge and literature on the chemical processes in typical aqueous processing of nuclear fuels. A long list of possible radionuclides present in irradiated fuel was generated and then trimmed by considering isotope half-life and calculating the dose from each to a maximum exposed individual with the US EPA airborne radiological dispersion and risk assessment code CAP88 (Rosnick 1992) to yield a short list of elements that actually need to be considered for control because they require high decontamination factors to meet a reasonable fraction of the regulated release. Each of these elements is then discussed with respect to what is known in the literature about their behavior in a reprocessing facility. The context for the evaluation in this document is a UO2-based fuel processed through an aqueous-based reprocessing system with a TBP-based solvent extraction chemistry. None of these elements form sufficiently volatile compounds in the context of the reprocessing facility to be of regulatory concern.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Threat Identification Parameters for a Stolen Category 1 Radioactive Source

Radioactive sources are used very widely for research and practical applications across medicine, industry, government, universities, and agriculture. The risks associated with these sources vary widely depending on the specific radionuclide used to make the source, source activity, and its chemical and physical form. Sources are categorized by a variety of classification schemes according to the specific risk they pose to the public. This report specifically addresses sources that are classified in the highest category for health risk (category 1). Exposure to an unshielded or lightly shielded category 1 source is extremely dangerous to life and health and can be fatal in relatively short exposure times measured in seconds to minutes. A Category 1 source packaged according to the guidelines dictated by the NRC and U.S. Department of Transportation will typically be surrounded by a large amount of dense shielding material, but will still exhibit a significant dose rate in close proximity. Detection ranges for Category 1 gamma ray sources can extend beyond 5000 ft, but will depend mostly on the source isotope and activity, and the level of shielding around the source. Category 1 sources are easy to detect, but difficult to localize. Dose rates in proximity to an unshielded Category 1 source are extraordinarily high. At distances of a few hundred feet, the functionality of many commonly used handheld instruments will be extremely limited for both the localization and identification of the source. Radiation emitted from a Category 1 source will scatter off of both solid material (ground and buildings) and the atmosphere, a phenomenon known as skyshine. This scattering affects the ability to easily localize and find the source.

07 ISOTOPE AND RADIATION SOURCES↗

DEPO-related to Radioactive Sources.

Design and Evaluation Process Outline (DEPO) is discussed as it pertains to protection of radioactive sources. The bulk of the report describes features of various kinds of detection systems, and follows this with systems for entry control and personnel identification.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Normalizing Radionuclide Concentration Exposure Rate and Dose Rate Data for the Effects of Radioactive Decay and Weathering Processes

This report describes the procedure that will be implemented to normalize radiological data, collected at various times, to one point in time. Raw radiological data is adjusted for the effects of radioactive decay and weathering processes. Normalizing the radiological data to one point in time enables data that has been collected at various times to be directly compared and utilized in radiological assessment, statistical analysis, and atmospheric dispersion models. This report fulfills a deliverable requirement for the U.S. Department of Energy’s, NA-84 Technology Integration Program for the FY17 project, SNL17-CM-635, Normalizing Radiological Data for Analysis and Integration into Models.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Radioactive Source Shielding Strategies

This report discusses different options for shielding radioactive sources that will be transported in the Ford Raptor with a stop box during source roundups in Inner Mongolia and aims to determine the best shield option. A packaging and shielding plan based on pre-recovery information is also suggested.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Evaluation of Anodized and Electroplated Radioactive Check Sources for Radiological Monitoring Instruments

Radioactive check sources are often used for source checking calibrated instruments to confirm accurate readings are obtained from radiological monitoring instruments. Because of the importance of check sources and their application, PNNL conducted a study to evaluate the effectiveness and accuracy of active sources produced using different construction methods. Eleven, randomly selected check sources of both anodized (five) and electroplated (six) construction were evaluated, along with their calculated decay curves, to determine how well they withstand consistent, multi-year use in the field. Results show that the anodized and electroplated check sources evaluated hold up well enough to continue their use, regardless of wear and tear sustained over years of use. This report provides the source information, empirical data for the 11 anodized and electroplated check sources and their representative decay curves, and it documents the conclusion that anodized and electroplated check sources are reliable for routine use in the field over multiple years.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radioactive Plume Avoidance and Aircraft Decontamination – Best Practices

Response to an incident involving the release of radioactive material will most likely involve aircraft for disaster relief and radiological monitoring. Aircraft flying into a radiologically contaminated area risk becoming contaminated, and in the worst cases having to be removed from service. Contamination is avoidable, and decontamination is possible, but both require planning and forethought.

61 RADIATION PROTECTION AND DOSIMETRY↗