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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Method and system for radioisotope generation

A system and a process for producing selected isotopic daughter products from parent materials characterized by the steps of loading the parent material upon a sorbent having a functional group configured to selectively bind the parent material under designated conditions, generating the selected isotopic daughter products, and eluting said selected isotopic daughter products from the sorbent. In one embodiment, the process also includes the step of passing an eluent formed by the elution step through a second sorbent material that is configured to remove a preselected material from said eluent. In some applications a passage of the material through a third sorbent material after passage through the second sorbent material is also performed.

42 ENGINEERING↗

Applications of Hyporheic Zone Sampling for Assessing VOC Plume Engineered Remediation and Natural Attenuation Effectiveness - 20414

Determining the efficacy of engineered remedial actions and/or natural attenuation as an acceptable EPA Record of Decision (ROD) must address long-term temporal and spatial variability. Since final plume downslope destinations are aquifers and related surface streams and rivers, hyporheic zone sampling is essential. Comprehensive hyporheic sampling documents plume groundwater remediation prior to upwelling into stream benthic strata and natural attenuation within this dynamic zone itself. Our intensive sampling of the Savannah River Site (SRS) Chemical, Metals, and Pesticides (CMP) Pits VOC plume-fringe from 2005 to 2018 documented PCE natural attenuation and effectiveness of In Situ Thermal Treatment (ISTT). Most plume hyporheic upwelling was delimited to a 20 m inflow reach along Pen Branch. Our study utilized corroborative sampling methodologies: ambient hole-water grab samples: passive diffusion bags (PDB); and hole-core sediment samples to confirm station to station spatial and temporal trends. VOC hot spot detections were confirmed from both groundwater and soil core samples. VOC pathways through the Pen Branch hyporheic zone were assessed at hole-installation using sequential soil samples from augered cores and grab-samples of hole-bottom water. Longer term, composite water samples were collected from PDBs deployed for a minimum two-week equilibration period. Soil samples were collected from the 15 and 65 cm core levels in December 2017 and June 2018 at six stations. Additional core depths of 40 and 85 cm were sampled in June 2018 at the highest VOC station (5DB80). All samples were analyzed in an EPA certified lab by purge and trap GC-MS. Effectiveness of previous ISTT and soil vapor extraction (SVE) for this CMP Pits PCE plume, was clearly documented by significant downward trends in VOC at hyporheic zone stations prior to December 2015. Achieving final stage conversions of PCE daughter products to ethene and CO{sub 2} may be limited depending upon suitable interactions between hyporheic zone sediment morphology, hydrology, and redox conditions. Because declines in VOC daughter products at our hyporheic stations may also be caused by physical actions of dilution and dispersion rather than true biochemical dechlorination, full quantification of natural attenuation requires the use of compound-specific isotope ratio analysis (CSIA) and microbial 16S rRNA with qPCR. To assist these next-phase efforts, a natural attenuation index (NAI) was used to help produce quicker, more cost-effective decision making for locating CSIA and microbial sampling efforts. The NAI used natural logarithm transformed GC-MS results for station VOC degradation compounds versus VOC parent compounds. Wide differences were observed between stations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radon Diffusion Measurement in Polyethylene based on Alpha Detection

We present a method to measure the diffusion of Radon in solid materials based on the alpha decay of the radon daughter products. In contrast to usual diffusion measurements which detect the radon that penetrates a thin barrier, we let the radon diffuse into the material and then measure the alpha decays of the radon daughter products in the material. We applied this method to regular and ultra high molecular weight poly ethylene and find diffusion lengths of order of mm as expected. However, the preliminary analysis shows significant differences between two different approaches we have chosen. These differences may be explained by the different experimental conditions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

238 PuO 2 Fuel and Dosimetry

238 Pu is an ideal material for use as a heat source with its half-life of 87.7 years and copious particle emissions. 238 Pu radioisotope thermoelectric generators (RTGs) have found use for pacemakers, Apollo Space missions, Mars rovers, and Voyager spacecraft. In evaluating the dose to personnel and components near a 238 Pu-based RTG, a number of additional nuclides and their daughter products must be considered to get an accurate estimate for γ-dose, and the amount of 17 O and 18 O for the neutron-dose must be considered. This paper looks at the contributing nuclides and their daughter products that add the most to the dose rates.

07 ISOTOPE AND RADIATION SOURCES↗

Fractionation of UF6 and daughter progeny in storage cylinders from external heating

Abstract Uranium hexafluoride (UF 6 ) is a significant concern for material accountancy and verification in the international safeguards community. Verification of the contents of UF 6 cylinders is generally attempted with gamma spectroscopy but the current methods assume a uniform, homogeneous UF 6 mass distribution within the cylinder. In this work, it was found experimentally and confirmed via modeling, that under an external heat load (the sun), the UF 6 and its daughter products undergo fractionation in the cylinder. This fractionation of the UF 6 and daughter products can cause an errant measurement of the enrichment of the cylinder when using the current verification methods.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Thermal impacts on nondestructive analysis measurements of uranium hexafluoride

A series of nondestructive assay measurements were performed before, during, and after localized heating of an industrial standard 12B cylinder of uranium hexafluoride to replicate dose variations previously observed on commercial 30B cylinders. While cylinders represent a closed system, enrichment measurements may be impacted by altered uranium and daughter product distributions due to sublimation. A series of measurements were performed to examine localized heating impacts on dose rates, ratios of uranium and daughter product distributions, and measured 235 U enrichment as calculated by two different approaches. The less complex enrichment meter approaches were found to be more robust and less prone to deviation than isotope ratio approaches such as FRAM, but the impact can be minimized by using observable dose changes to avoid impacted areas.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Removal of radionuclides from acidic solution by activated carbon impregnated with methyl- and carboxy-benzotriazoles

The removal efficiencies of metals commonly used to model the fate and transport of aqueous uranium and radioactive its daughter products, were observed on activated carbons impregnated with different benzotriazole derivatives. Acidic solutions containing U(VI), Sr(II), Eu(III), and Ce(III) were used to determine the immobilization potential of carboxybenzotriazole (CBT) and methylbenzotriazole (MeBT), where these derivatives were sorbed to different types of granular activated carbon (GAC). This sorption behavior can be predicted by Redlich–Peterson model. Flow-through column tests showed that the immobilization of uranium and some of its daughter products, significantly improves in response to oxidized GACs saturated with carboxybenzotrzole (CBT), which reached a maximum elimination for U(VI) at 260 BV, Eu(III) at 114 BV, Ce(III) at 126 BV, and Sr(II) at 100. MeBT significantly desorbed from GAC under acidic conditions. Trace amounts of CBT were observed in some column effluents, but this did not appear to alter the effectiveness of metal removal, regardless of the model radionuclide studied. These results suggest that enhanced immobilization of selected metals on GAC, can be achieved by impregnating oxidized activated carbon with carboxylated benzotriazoles, and that metal removal efficiency on this media, is related to their valence and ionic radius in acidic environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solving Complex Radioactive Decay Chains for Future Assessment and Cleanup Decisions - 17046

In support of U.S. Environmental Protection Agency's on-line calculators for risk and dose assessment, a decay chain tool was developed to address the need to understand how radionuclide activity changes with time as the activity measured in the past will be different from current and future levels. When a radionuclide decays, its activity decreases exponentially as a function of time transforming into a different atom - a decay product. The atoms keep transforming to new decay products until they reach a stable state and are no longer radioactive. The series of decay products created to reach this balance is called the decay chain. For radionuclide chains, the daughter products can have significant implications in dosimetry and remediation. Thus, risk assessors evaluating sites with radioactive contamination need to plan for future progeny ingrowth, in addition to sampled radionuclides. These are important considerations for risk quantification during the characterization and cleanup plans, particularly when sampling may have occurred years before the remediation cleanup work begins. If a radionuclide half-life and current activity are known, then hand-calculating the future activity is straightforward. However, calculating the ingrowth of progeny quickly becomes cumbersome for longer chains such as the Thorium-232 decay series. For the more complex chains where many daughters are formed, possibly with multiple branches, this calculation involves solving a complex set of simultaneous differential equations known as the Bateman Equation. The Decay Chain Activity Projection Tool calculates the activity of radionuclides and their progeny as a function of time. This tool currently uses a combination of Perl, JavaScript, Plot.ly, and jQuery to automatically construct the radionuclide decay chains, solve the resulting Bateman Equation, and provide the user with tabular solution output and plots. Additional software may be used as development advances. The risk assessor can then use the data for exposure assessment and cleanup decisions without further costly sampling. The benefits of providing this calculator are to prevent overestimation of risk due to decay of the parent isotope and to avoid underestimation of risk due to ingrowth of progeny more toxic than the parent. Graphs are provided to show the simultaneous decay rates and ingrowth, as well as tabular output at time-point T and all the decay half-life intervals. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Treatability Study for Edible Oil Deployment for Enhanced cVOC Attenuation for T-Area, Savannah River Site

Groundwater beneath T-Area, a former laboratory and semiworks operation at the Department of Energy (DOE) Savannah River Site (SRS), is contaminated by chlorinated solvents (cVOCs). Since the contamination was detected in the 1980s, the cVOCs at T-Area have been treated by a combination of soil vapor extraction and groundwater pump and treat. The site received approval to temporarily discontinue the active groundwater treatment and implement a treatability study of enhanced attenuation - an engineering and regulatory strategy that has recently been developed by DOE and the Interstate Technology and Regulatory Council (ITRC 2007). Enhanced attenuation uses active engineering solutions to alter the target site in such a way that the contaminant plume will passively stabilize and shrink and to document that the action will be effective, timely, and sustainable. The paradigm recognizes that attenuation remedies are fundamentally based on a mass balance. Thus, long-term plume dynamics can be altered either by reducing the contaminant loading from the source or by increasing the rate of natural attenuation processes within all, or part of, the plume volume. The combination of technologies that emerged for T-Area included: (1) neat (pure) vegetable oil deployment in the deep vadose zone in the former source area, (2) emulsified vegetable oil deployment within the footprint of the groundwater plume, and (3) identification of attenuation mechanisms and rates for the distal portion of the plume. In the first part, neat oil spreads laterally forming a thin layer on the water table to intercept and reduce future cVOC loading (via partitioning) and reduce oxygen inputs (via biostimulation). In the second and third parts, emulsified oil forms active bioremediation reactor zones within the plume footprint to degrade existing groundwater contamination (via reductive dechlorination and/or cometabolism) and stimulates long-term attenuation capacity in the distal plume (via cometabolism). For TArea, the enhanced attenuation development process proved to be a powerful tool in developing a strategy that provides a high degree of performance while minimizing adverse collateral impacts of the remediation (e.g., energy use and wetland damage) and minimizing life-cycle costs. As depicted in Figure 1, Edible oil deployment results in the development of structured geochemical zones and serves to decrease chlorinated compound concentrations in two ways: (1) physical sequestration, which reduces effective aqueous concentration and mobility; and (2) stimulation of anaerobic, abiotic and cometabolic degradation processes. In the central deployment area, contaminant initially partitions into the added oil phase. Biodegradation of the added organic substrate depletes the aquifer of oxygen and other terminal electron acceptors and creates conditions conducive to anaerobic degradation processes. The organic substrate is fermented to produce hydrogen, which is used as an electron donor for anaerobic dechlorination by organisms such as Dehalococcoides. Daughter products leaving the central treatment zone are amenable to aerobic oxidation. Further, the organic compounds leaving the central deployment zone (e.g., methane and propane) stimulate and enhance down gradient aerobic cometabolism which degrades both daughter compounds and several parent cVOCs. Figure 1 depicts TCE concentration reduction processes (labeled in green) along with their corresponding breakdown products in a structured geochemical zone scenario. A consortium of bacteria with the same net effect of Dehalococcoides may be present in the structured geochemical zones leading to the degradation of TCE and daughter products. Figure 2 shows a schematic of the documented cVOC degradation processes in both the anaerobic and aerobic structured geochemical zones. Specific aerobic and anaerobic bacteria and their degradation pathways are also listed in the diagram and have either been confirmed in the field or the laboratory. See references in the bibliography in Section 11.

54 ENVIRONMENTAL SCIENCES↗

Daughters mimic sterile neutrinos (almost!) perfectly

Since only recently, cosmological observations are sensitive to hot dark matter (HDM) admixtures with sub-eV mass, m{sub hdm}{sup eff} < eV, that are not fully-thermalised, Δ N{sub eff} < 1. We argue that their almost automatic interpretation as a sterile neutrino species is neither from theoretical nor practical parsimony principles preferred over HDM formed by decay products (daughters) of an out-of-equilibrium particle decay. While daughters mimic sterile neutrinos in N{sub eff} and m{sub hdm}{sup eff}, there are opportunities to assess this possibility in likelihood analyses. Connecting cosmological parameters and moments of momentum distribution functions, we show that—also in the case of mass-degenerate daughters with indistinguishable main physical effects—the mimicry breaks down when the next moment, the skewness, is considered. Predicted differences of order one in the root-mean-squares of absolute momenta are too small for current sensitivities.

79 ASTRONOMY AND ASTROPHYSICS↗

Application of Biodegradable Oils (VOS{sup TM}) for Treatment of Chlorinated Ethenes in the Vadose Zone - 12085

Few active remediation alternatives are available to treat residual chlorinated volatile organic compounds (cVOCs) within the vadose zone. Soil vapor extraction (SVE) can be very effective at removing cVOCs in permeable soils; however, recoveries decline substantially in low permeability zones where mass transfer is diffusion-limited. Entrapped cVOCs in these zones represent a slow but continuous source of contamination to underlying groundwater. An ongoing field study was initiated at the Department of Energy's Savannah River Site (SRS) to evaluate an in situ biological treatment technology to address cVOC contamination in the vadose zone. Developed by Savannah River National Laboratory (SRNL), VOS{sup TM} is a thixotropic (shear thinning) formulation of biodegradable oil, water, nutrients, buffers, and de-chlorinating bacteria (Dehalococcoides sp.) that is designed to sequester and biodegrade slow-diffusing cVOCs from unsaturated, low permeable soils. Injection of 871 L (230 gal) of VOS{sup TM} resulted in a rapid and significant decrease in cVOC gas concentration, generation of cVOC daughter products, a decrease in oxygen concentration, and an increase in carbon dioxide and methane production. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

LaPO4 Nanoparticles Doped with Actinium-225 that Partially Sequester Daughter Radionuclides

Nanoscale materials have been envisioned as carriers for various therapeutic drugs, including radioisotopes. Inorganic nanoparticles (NPs) are particularly appealing vehicles for targeted radiotherapy because they can package several radioactive atoms into a single carrier and can potentially retain daughter radioisotopes produced by in vivo generators such as actinium -225 (225Ac, t1/2=10 d). Decay of this radioisotope to stable bismuth-209 proceeds through a chain of short-lived daughters accompanied by the emission of four -particles that release >27 MeV of energy. The challenge in realizing the enhanced cytotoxic potential of in vivo generators lies in retaining the daughter nuclei at the therapy site. When 225Ac is attached to targeting agents via standard chelate conjugation methods, all of the daughter radionuclides are released after the initial -decay occurs. In this work, 225Ac was incorporated into lanthanum phosphate NPs to determine whether the radioisotope and its daughters would be retained within the dense mineral lattice. Further, the 225Ac-doped NPs were conjugated to the monoclonal antibody mAb 201B, which targets mouse lung endothelium through the vasculature, to ascertain the targeting efficacy and in vivo retention of radioisotopes. Standard biodistribution techniques and microSPECT/CT imaging of 225Ac as well as the daughter radioisotopes showed that the NPs accumulated rapidly in mouse lung after intravenous injection. By showing that excess, competing, uncoupled antibodies or NPs coupled to control mAbs are deposited primarily in the liver and spleen, specific targeting of NP-mAb 201B conjugates was demonstrated. Biodistribution analysis showed that ~30% of the total injected dose of La(225Ac)PO4 NPs accumulated in mouse lungs 1 h post-injection yielding a value of % ID/g >200. Furthermore, after 24 h, 80% of the 213Bi daughter produced from 225Ac decay was retained within the target organ and 213Bi retention increased to ~87% at 120 h. In vitro analyses, conducted over a one month interval demonstrated that ~50% of the daughter was retained within the La(225Ac)PO4 NPs at any time over that time frame. Although most of the -rays from radionuclides in the 225Ac decay chain are too energetic to be captured efficiently by SPECT detectors, appropriate energy windows were found that provided dramatic microSPECT images of the NP distribution in vivo. We conclude that La(225Ac)PO4 mAb conjugates can be targeted efficiently to mouse lung while partially retaining daughter products and that targeting can be monitored by biodistribution techniques and microSPECT imaging.

60 APPLIED LIFE SCIENCES↗

Microbeam, timing and signal-resolved studies of nuclear materials with synchrotron X-ray sources

The development of ultra-brilliant synchrotron X-ray sources enables characterization methods that are particularly important for nuclear materials. Here we discuss emerging synchrotron methods with unprecedented signal-to-noise, spatial and time resolution. Microprobe methods are discussed that extend virtually any X-ray characterization measurement to ultra-small sample volumes. This ability is critical to resolve heterogeneities in nuclear materials and for studies on volumes with vastly lower activity than are needed for traditional X-ray characterization. Specific methods discussed include microdiffraction for the characterization of local crystal structure and micro-spectroscopy techniques that allow for characterization of elemental distributions with sensitivity for daughter products, oxidation states and diffusion through buffer layers. Opportunities are also discussed that exploit the high brilliance and pulsed nature of synchrotron radiation to reduce backgrounds from sample radiation and to study materials dynamics.

36 MATERIALS SCIENCE↗

Guidance on Radiochronometry

Radiochronometry is the measurement of radioactive materials and their decay products to determine the “age” of the material. It differs from the practice of geochronology in that the materials (samples) are man-made, and in that the timespan of interest is confined to the nuclear era, i.e., since the discovery of fission in 1939. In radiochronometry, the “age” of the material ideally records the time when the sample was manufactured, or produced in the final form that is analyzed in the laboratory. It is an important predictive signature in a nuclear forensic investigation which can help in the attribution to a source. The calculation of this “age” can only be made if a model is invoked that allows simplification of the parent radionuclide to daughter isotope decay equation. The simplification required for this model is that the parent was purified completely from all traces of its daughter product at the time of sample preparation. Then, this “age” should be described as the “model age” from which a “model date” in the past can then be calculated. For this model date to represent the date of sample preparation, two other assumptions are required to be true. The first is that the material has remained a closed system since that time (i.e., that there has been no loss or gain of either parent or daughter), and the second is that the analyses are accurate.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Demonstration of Combined Zero-Valent Iron and Electrical Resistance Heating for In Situ Trichloroethene Remediation

The effectiveness of in situ treatment using zero-valent iron to remediate sites with non-aqueous phase or significant sediment-associated contaminant mass can be limited by relatively low rates of mass transfer to bring contaminants in contact with the reactive media. For a field test in a trichloroethene source area, combining moderate-temperature (maximum 50oC) subsurface electrical resistance heating with in situ ZVI treatment was shown to accelerate dechlorination and dissolution rates by a factor of 4 to 6 based on organic daughter products and a factor 8-16 using a chloride concentrations. A mass-discharge-based analysis was used to evaluate reaction, dissolution, and volatilization at ambient groundwater temperature (~10oC) and as temperature was increased up to about 50oC. Increased reaction and contaminant dissolution were observed with increased temperature, but volatilization was minimal during the test because in situ reactions maintained low aqueous-phase TCE concentrations.

54 ENVIRONMENTAL SCIENCES↗

The estimation of absorbed dose rates for non-human biota : an extended inter-comparison.

An exercise to compare 10 approaches for the calculation of unweighted whole-body absorbed dose rates was conducted for 74 radionuclides and five of the ICRP's Reference Animals and Plants, or RAPs (duck, frog, flatfish egg, rat and elongated earthworm), selected for this exercise to cover a range of body sizes, dimensions and exposure scenarios. Results were analysed using a non-parametric method requiring no specific hypotheses about the statistical distribution of data. The obtained unweighted absorbed dose rates for internal exposure compare well between the different approaches, with 70% of the results falling within a range of variation of {+-}20%. The variation is greater for external exposure, although 90% of the estimates are within an order of magnitude of one another. There are some discernible patterns where specific models over- or under-predicted. These are explained based on the methodological differences including number of daughter products included in the calculation of dose rate for a parent nuclide; source-target geometry; databases for discrete energy and yield of radionuclides; rounding errors in integration algorithms; and intrinsic differences in calculation methods. For certain radionuclides, these factors combine to generate systematic variations between approaches. Overall, the technique chosen to interpret the data enabled methodological differences in dosimetry calculations to be quantified and compared, allowing the identification of common issues between different approaches and providing greater assurance on the fundamental dose conversion coefficient approaches used in available models for assessing radiological effects to biota.

59 BASIC BIOLOGICAL SCIENCES↗

A low abundance of “{sup 35}cs in the early solar system from barium isotopic signatures of volatile-depleted meteorites

Precise knowledge of the abundances of short-lived radionuclides at the start of the solar system leads to fundamental information about the stellar environment of solar system formation. Previous investigations of the short-lived {sup 135}Cs →{sup 135}Ba system (t {sub 1/2} = 2.3 Ma) have resulted in a range of calculated initial amounts of {sup 135}Cs, with most estimates elevated to a level that requires extraneous input of material to the protoplanetary disk. Such an array of proposed {sup 135}Cs/{sup 133}Cs initial solar system values has severely restricted the system’s use as both a possible chronometer and as an informant about supernovae input. However, if {sup 135}Cs was as abundant in the early solar system as previously proposed, the resulting deficits in its daughter product {sup 135}Ba would be easily detectable in volatile-depleted parent bodies (i.e., having sub-chondritic Cs/Ba) from the very early solar system. In this work, we show that angrites and eucrites, which were volatile-depleted within ∼1 million years of the start of the solar system, do not possess deficits in {sup 135}Ba compared to other planetary bodies. From this, we calculate an upper limit for the initial {sup 135}Cs/{sup 133}Cs of 2.8 × 10{sup −6}, well below previous estimates. This significantly lower initial {sup 135}Cs/{sup 133}Cs ratio now suggests that all of the {sup 135}Cs present in the early solar system was inherited simply from galactic chemical evolution and no longer requires an addition from an external stellar source such as an asymptotic giant branch star or SN II, corroborating evidence from several other short-lived radionuclides.

79 ASTRONOMY AND ASTROPHYSICS↗

Contaminant Migration Modeling to Support the In Situ Decommissioning of Hardened Nuclear Facilities - 20215

The decommissioning of hardened nuclear facilities provides a unique challenge in balancing current worker dose with exposure to future receptors and media. In situ decommissioning (ISD) is a cost-effective and safe option for the closure of such facilities but requires a detailed understanding of the threat that radioactive and hazardous constituents remaining in the facilities pose to groundwater and surrounding surface water. The Savannah River Site (SRS) extensively employs contaminant migration models within the decommissioning process to develop site-specific removal, grouting, and monitoring strategies in support of safe and effective final end states of nuclear facilities. This work discusses the use of contaminant migration modeling in the ISD process at SRS, including specific examples from the closure of P-Reactor and R-Reactor, Building 235-F, F-Canyon and F/H Laboratory Complex. Migration models developed during the closure of P-Reactor and R-Reactor were divided into four source areas: the reactor vessel, the process area, the disassembly basin, and the purification wing. Each source area was assigned a specific inventory and migration pathway and was then subject to varying hypothetical removal, capping, and grouting schemes. Modeling indicated that groundwater Maximum Concentration Limits (MCLs) might be exceeded if no action was taken for eleven and ten constituents of concern (COCs) at P-Reactor and R-Reactor, respectively. These exceedances could occur in as few as 200 to 500 years. Alternatively, the migration modeling demonstrated that the selected ISD actions reduced contaminant mobility which allowed for significant radioactive decay and resulted in fewer predicted exceedances of groundwater MCLs (five COCs for P-Reactor; eight COCs for R-Reactor). In response to the modeling results for P-Reactor and R-Reactor, effectiveness monitoring programs were developed to target contaminants, specific to each reactor, that may migrate to groundwater. Contaminant migration modeling also revealed that roof collapse was a large factor in the release of COCs to the environment, giving rise to roof improvements, and an inspection and vegetation control program to ensure roof stability over time. Contaminant migration modeling is also aiding in the closure planning for hardened facilities in F Area. Building 235-F housed the Actinide Billet Line, which produced Np-237 billets for irradiation in SRS reactors, and the Plutonium Fuel Form (PuFF) facility that produced Pu-238 heat sources for the space program. As a result of these missions, areas within Building 235-F contain considerable residual amounts of both Pu-238 and Np-237. Contaminant migration modeling of Building 235-F was originally performed in 2012 to identify the feasibility of ISD and the amount of radioactive material removal required to prevent the exceedance of groundwater MCLs. The original model indicated that a 60% reduction in the PuFF facility Pu-238 inventory could keep groundwater concentrations below standards, while Np-237 did not pose a threat to groundwater. However, updates to the model with an emphasis on source impact pathways revealed that, due to the orientation of the source areas relative to groundwater flow, no amount of reasonable removal of Pu-238 would keep groundwater concentrations below MCLs and that Np-237 could be a large contributor to localized MCL exceedances. With this insight, the refined 2019 model is being used to assist in the development of grouting plans specific to each facility source area, where bentonite may be utilized to slow the migration of Pu-238 and its daughter products from the PuFF facility and a reducing grout may decrease Np-237 transport by ensuring the nuclide remains in the less mobile +IV oxidation state. The beginning phases of contaminant migration modeling are underway for F-Canyon and associated facilities using lessons learned from the Reactors and Building 235-F. A contaminant migration pathway, similar to the pathway used for the reactor vessels, is being developed for the hot and warm canyons. The F-Canyon inventories are being spatially refined to identify specific and localized source zones, comparable to Building 235-F, that may impact groundwater. Contaminant migration modeling provides vital input within the ISD process, from facility investigation to post closure effectiveness monitoring, making it a valuable tool in the development of safe and effective end states for hardened nuclear facilities at SRS. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗