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Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Since 1952, liquid radioactive effluent containing 238-242 Pu, 241 Am, 237 Np, 137 Cs, and 99 Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Here, leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Molten Salt Tritium Transport Experiment: A Versatile Fluoride Salt Loop for Validation of Tritium Transport Phenomena

Tritium is generated in Molten Salt Reactors (MSRs) from neutron capture by lithium and other constituents of the molten salt FLiBe. Tritium is a unique radionuclide as it readily permeates through hot structural materials. Thus, any material in contact with tritium laden molten salt is a potential pathway for release. Understanding tritium transport and devising adequate control strategies is necessary for the safe operation of MSRs. The Molten Salt Tritium Transport Experiment (MSTTE) is a forced-convection fluoride salt loop with the capability to inject hydrogen isotopes into flowing molten salt and to measure transport phenomena such as permeation through metals and evolution from free-surfaces. MSTTE is designed to be versatile to test potential control technology in future campaigns. This report focuses on the current design and analysis of MSTTE. Custom designed and fabricated experiment components such as the hydrogen injection system, permeation test section, diagnostics, and gas distribution system are discussed in detail. System-level tritium transport modeling using the System Analysis Module investigates experiment parameters such as hydrogen source terms, salt flow rate, and salt temperature. Computational fluid dynamics of the salt flow in the permeation test section informs design choices to establish fully developed flow in the measured permeation zone.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

235-F GoldSim Fate and Transport Model: Uncertainty Quantification

Building 235-F was configured with two missions in mind: Actinide Billet Line (ABL) and the fabrication of Pu-238 oxide for space program applications. ABL produced Np-237 billets for use in SRS reactors, whereas the design process, fabrication, and examination of Pu-238 oxide powder occurred within the following areas, respectively: Plutonium Experimental Facility (PEF), Plutonium Fuel Form (PuFF), and Old Metallography Lab (OML). By 1990 production ceased and by 2006 de-inventory occurred; however, assays have shown significant holdup remains within ABL and PuFF. As a result, 235-F is a Category 2 nuclear facility, with plans to undergo deactivation and decommission (D and D) via In-Situ Disposal (ISD). The purpose of this project is to ensure United States Environmental Protection Agency (USEPA) groundwater radiation maximum contaminant level (MCL) and dosage standards are met during the D and D of 235-F by quantifying uncertainty through probabilistic modeling and evaluation of various ISD alternatives. GoldSim is a dynamic modeling software package with a graphical, object-oriented interface capable of capturing the influence of complex system input variability on probabilistic system outcomes. A GoldSim stochastic fate and transport model for 235-F was developed and matched with a PORFLOW deterministic model to simulate probabilistic release and flow of radionuclides from ABL and PuFF into the vadose zone, the Upper Three Runs (UTR) Aquifer, and UTR Creek. The GoldSim model was used to probabilistically evaluate four ISD scenarios against USEPA groundwater radiation MCLs and dosage standards. The deterministic 235-F GoldSim fate and transport model continues to be refined to match the results of the PORFLOW deterministic model to ensure the model accurately represents radionuclide movement through the groundwater system. The stochastic variables that are utilized within the GoldSim model are founded on the most current data; a conservative perspective is taken where needed. Alignment with the PORFLOW deterministic model, coupled with input stochastic variability, allows the probabilistic 235-F GoldSim model to capture the conservative breadth of possible outcomes for radionuclide fate within this particular system. This ensures that the USEPA MCLs and dosage limits hold even in the worst case scenarios.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Calculations versus measurements for residual dose rates from SNS spent structures

Here, residual dose rate measurements were conducted on target vessel #13 and proton beam window #5 after extraction from their service locations. These measurements are used to verify calculation methods of radionuclide inventory assessment that are typically performed for nuclear waste characterization and transportation of these structures. Neutronics analyses for predicting residual dose rates are carried out using the transport code MCNPX and the transmutation code CINDER90. For transport analyses a complex and rigorous geometry model of the structures and their surroundings are applied. The neutronics analyses are carried out using the Bertini and CEM high energy physics models for simulating particles interactions above the table-based cross section range. Finally, obtained calculational results are analyzed and compared to the measured dose rates and overall show good agreement within 25%, which shows applicability of the methods used in analyses.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

General overview of multiphysics modeling and simulation at CEA/DES/IRESNE supporting safety, operating and development of nuclear reactors and facilities

This paper presents a general overview of the innovative multiphysics research/development activities carried on by the CEA/DES/IRESNE institute. Eight main different multiphysics fields addressed by IRESNE have been listed (among others: fuel fabrication, behavior of fuels, of reactors, of corium, radionuclide transfer to environment,...) in relation with the involved coupled physics: neutron transport, fluid mechanics, electro-magnetism, heat transfer, solid mechanics and (physico-)chemistry. The major mission of IRESNE institute is to study current and future nuclear systems integrated into a low carbon energy system. To fulfill this mission, IRESNE's activities rely on the development and the implementation of multiphysics modeling, advanced coupling scheme, data transfer techniques and dedicated multiphysics experimentations. Indeed, such multiphysics simulation approach of nuclear systems is today required to deal with the complex intrinsic features of studied phenomena. This approach aims at taking into account physical phenomena interactions, at each interest modeling scale, in order to reach an accurate and predictive behavior representation of a system component or of the whole system. The final objective is to contribute to the development of digital reactor, core and fuel at CEA, by progressing on applied mathematics, high-performance computing and physical mechanism understanding.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Fate and transport of unruptured tri-structural isotropic (TRISO) fuel particles in the event of environmental release for advanced and micro reactor applications

Advanced nuclear reactor designs and advanced fuel types offer safety features that may reduce environmental consequences in an accident scenario when compared to conventional reactors and fuels. One advanced reactor fuel is tri-structural isotropic (TRISO) fuel particles which are approximately 0.9 mm in diameter. TRISO particle mobility, assuming the particle is unruptured and the encapsulated radionuclides are contained, was explored through a theoretical examination of mobility through atmospheric, soil and groundwater, surface water, and non-human biota transport pathways. TRISO particles are too large and dense to travel in the atmosphere except under extreme conditions. TRISO particles are too large to penetrate most soil profiles and so cannot be transported with groundwater. TRISO particles will settle out of the water column in surface waters but the transport will depend on the energy of the body of water and likelihood of extreme dispersion events. TRISO particles could be transported by non-human biota. The size of TRISO particles could allow them to be intentionally moved by non-human biota if they are ingested as a gastrolith or if they are mistaken for something in the organism’s diet. Generally, TRISO particles will have reduced environmental mobility compared to releases of radionuclides in the event of an accident in a conventional nuclear reactor. The extent of transport has implications in emergency planning zone designations and other considerations for licensing and deploying TRISO-fueled reactors. Finally, further research and experimental work exploring TRISO particle mobility is required to understand the full environmental mobility of TRISO particles.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Modeling Interfaces to Support Low-Level Waste Disposal System Performance Assessments - 20366

In low-level waste (LLW) disposal sites, interfaces between cementitious materials, used as waste forms and/or engineered barriers, and the surrounding soil or backfill material are often encountered. Reactions across these interfaces may lead to chemical and structural alteration of the cementitious and backfill materials that may ultimately affect long-term performance. For example, the ingress of carbon dioxide from soil gas into a waste tank concrete shell at the Hanford Site or Savannah River Site (SRS) or a low-level waste disposal vault at SRS leads to carbonation of cement hydration products (e.g. portlandite, calcium-silicate hydrate or C-S-H, and ettringite). The result of carbonation is a decrease in pH in the cement paste portion of the tank wall or vault concrete structure that could ultimately lead to de-passivation of the embedded structural steel and, eventually, to cracking. Cracking can lead to increased ingress of water into the structure, corresponding increased release of constituents of concern, and to subsequent increased transport of these constituents to the surrounding environment. The mobility of trace constituents (e.g., radionuclides of concern) in waste forms may increase in response to changes in pH, pore structure, and mineralogical gradients. Depletion of portlandite results in subsequent decalcification of C-S-H that leads to changes in the cement strength and may lead to structural failure. At the boundary between waste forms and concrete vaults, the migration of sulfate ions from the salt waste form (e.g., the saltstone waste form used for LLW disposal at the Savannah River Site in Saltstone Disposal Units, or SDUs) into the barrier or vault concrete has been predicted to result in expansive mineral phase formation (or 'sulfate attack'). Expansive mineral formation could result in cracking and potential loss of structural integrity in the vault concrete. In the performance assessment (PA) for the SRS SDUs, prediction of both the carbonation and sulfate attack fronts are critical to assessing the long-term performance of these LLW disposal vaults. A general purpose geochemical reactive transport model has been developed in LeachXS/ORCHESTRA to evaluate typical interfaces for LLW disposal environments, including SDUs at SRS. The model may be used to predict the long-term performance of interfaces between cementitious materials and saltstone or backfill materials with respect to primary phases by considering mass transport, cement chemistry, geochemical speciation, and multi-ionic diffusion over interfaces between different materials. The present study compares the performance and interactions between vault concrete and saltstone waste form for a representative SDU scenario. The materials were characterized using pH-dependence leaching test (EPA 1313) and semi-dynamic transport tests (EPA 1315) with test results used to parameterize the interface model. The development of a credible inter model provides an important basis for supporting future PAs where carbonation and sulfate attack are important aging and degradation mechanisms. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Integrated Security-Safety Consequence Study of a Heat Pipe Reactor

This report presents a preliminary demonstration of integrated security/safety consequence modeling to support potential physical security exemption justifications under the new Title 10 Code of Federal Regulations Part 53 licensing pathway, which allows exemptions if sabotage-induced radiological consequences do not exceed 25 rem at the site boundary two hours after release without mitigative actions. A hypothetical heat pipe microreactor subjected to direct sabotage by a 150 lbs. TNT-equivalent high-explosive device was analyzed using a simplified radionuclide release estimate based on DOE-HDBK-3010-94, implemented in the MELCOR severe accident analysis code to model release transport and attenuation through reactor/building compartments, with MELCOR outputs coupled to MACCS to compute offsite doses and the distance-to-threshold metric D 25rem . Six scenarios were evaluated to examine sensitivities to release pathway/building configuration and radionuclide form (vapor versus aerosols with different size distributions). Results show a positive correlation between leak path factor and D 25rem and indicate that reactor building compartmentalization can substantially reduce consequences (a single-story configuration reduced D 25rem by roughly an order of magnitude relative to a cavity-only configuration), while vapor versus aerosol assumptions had limited impact for the modeled two-story case on the spatial grid used.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Design of Instrumentation for Noble Gas Transport in LSTL Needed for Model Development

Development of molten salt reactors (MSRs) requires consideration of several physical phenomena that are different from the light water reactor (LWR) experience. While small-scale tests have been performed to understand the behavior of molten salts, the scale-up to larger experiments is an important step in the development of MSR designs. These small-scale experiments have given information on the thermodynamic state of the heat transport fluid and its constituents, thermophysical properties, convective flow, and corrosion. As detailed models have been developed, using these models to simulate larger scale experiments must incorporate physics that becomes important during scale-up, temperature inhomogeneities, complex flow behavior, and two-phase flow. The purpose of the work package has been to link experimental and modeling efforts in the support of licensing development to design and evaluate technologies to mitigate radionuclide release from MSRs. There were two main activities in this work package—one investigating fission product transport into the cover gas and the other on fission gas transport in the molten salt.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Considerations for Managing DOE Standard Canisters within an Over-canister as Part of an Integrated Waste Management System

To better enable informed decision making regarding the back end of the nuclear fuel cycle, the Integrated Waste Management Program within the U.S. Department of Energy, Office of Nuclear Energy (DOE-NE) has been sponsoring the research into a comprehensive integrated waste management system (IWMS) that considers all major back-end aspects of the nuclear fuel cycle (i.e., transportation, storage, and disposal). An important aspect of the IWMS is DOE-managed SNF. DOE and its predecessor agencies have generated, transported, received, stored, and reprocessed SNF at DOE facilities nationwide, and DOE is responsible for managing the SNF currently in its possession. These fuels come from a wide range of reactor types that employ various cladding materials, fuel materials, and enrichments. To enable interim, road-ready dry storage (RRDS) of the wide variety of SNF types found in the DOE inventory, a standardized canister system (i.e., the DOE Standard Canister) was proposed. This robust, welded canister system is designed to confine radionuclides, prevent criticality by precluding content moderation, and satisfy other requirements as part of a larger storage, transportation, and disposal system. While SNF has yet to be loaded into a DOE Standard Canister, DOE Standard Canister designs were included in past storage facility and disposal facility design licensing endeavors. In a renewed effort to evaluate packaging SNF at Idaho National Laboratory (INL) in a RRDS configuration, researchers are planning the RRDS Packaging Demonstration. This demonstration is supplemented by analytical structural, criticality, and material compatibility evaluations that support management of SNF in DOE Standard Canisters, taking advantage of past analysis work to the extent possible. One of the largest differences between the current Packaging Demonstration and past analytical evaluations is the inclusion of an over-canister containing multiple DOE Standard Canisters. For the Packaging Demonstration, DOE Standard Canisters loaded with SNF are planned to be placed in a larger diameter over-canister. The sealed over-canister could then be placed in a storage overpack for onsite storage, or in a transportation overpack for shipment to an offsite storage location or disposal site once one becomes available. This paper examines the relevant considerations and provides a preliminary evaluation of integrating the over-canister configuration into the storage, transportation, and disposal processes of the overall waste management system. For storage and transportation, the over-canister can be considered analogous to a multi-purpose canister (MPC) for commercial SNF. For disposal, the DOE Standard Canisters could be removed from the over-canister and placed in a co-disposal waste package with canisters containing vitrified HLW similar to configurations examined previously, or the sealed over-canisters might be capable of direct disposal in a waste package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Considerations for Managing DOE Standard Canisters within an Over-canister as Part of an Integrated Waste Management System PPT

To better enable informed decision making regarding the back-end of the nuclear fuel cycle, the Integrated Waste Management Program within the U.S. Department of Energy, Office of Nuclear Energy (DOE-NE) has been sponsoring research into a comprehensive integrated waste management system (IWMS) that considers all major back-end aspects of the nuclear fuel cycle (i.e., transportation, storage, and disposal). An important aspect of the IWMS is DOE-managed Spent Nuclear Fuel (SNF). DOE and its predecessor agencies have generated, transported, received, stored, and reprocessed SNF at DOE facilities nationwide, and DOE is responsible for managing the SNF currently in its possession. These fuels come from a wide range of reactor types that employ various cladding materials, fuel materials, and enrichments. To enable interim, road-ready dry storage (RRDS) of the wide variety of SNF types found in the DOE inventory, a standardized canister system (i.e., the DOE Standard Canister) was proposed for the packaging demonstration. This robust, welded canister system is designed to confine radionuclides, prevent criticality by precluding content moderation, and satisfy other requirements as part of a larger storage, transportation, and disposal system. While SNF has yet to be loaded into a DOE Standard Canister, DOE Standard Canister designs were included in past storage facility and disposal facility design licensing endeavors. In a renewed effort to evaluate packaging SNF at Idaho National Laboratory (INL) in a RRDS configuration, researchers are planning the RRDS Packaging Demonstration. This demonstration is supplemented by analytical structural, criticality, and material compatibility evaluations that support management of SNF in DOE Standard Canisters, taking advantage of past analysis work to the extent possible. One of the largest differences between the current Packaging Demonstration and past analytical evaluations is the inclusion of an over-canister containing multiple DOE Standard Canisters. For the Packaging Demonstration, DOE Standard Canisters loaded with SNF are planned to be placed in a larger diameter over-canister. The sealed over-canister could then be placed in a storage overpack for onsite storage, or in a transportation overpack for shipment to an offsite storage location or disposal site once one becomes available. This paper examines the relevant considerations and provides a preliminary evaluation of integrating the over-canister configuration into the storage, transportation, and disposal processes of the overall waste management system. For storage and transportation, the over-canister can be considered analogous to a multi-purpose canister (MPC) for commercial SNF. For disposal, the DOE Standard Canisters could be removed from the over-canister and placed in a co-disposal waste package with canisters containing vitrified high-level radioactive waste (HLW) similar to configurations examined previously, or the sealed over-canisters might be capable of direct disposal in a waste package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Influence of background sources and topographic resolution in the Weather Research and Forecasting Model on xenon plume characteristics at monitoring stations

For many atmospheric monitoring applications, networks of measurement sites—such as the radionuclide stations of the International Monitoring System—can be sparse. With measurement locations potentially hundreds to thousands of kilometers from a release it is important to quantify the effects of physical processes on transport and dispersion of plumes between source and measurement locations. This study addresses the effects of background sources and topography resolution near the release location of radionuclides. We use the Weather Research and Forecasting (WRF) model with inline chemistry to investigate (1) how an additional, time-varying source of 133 Xe, such as an operational medical isotope production facility, contributes to activity concentration measurements at monitoring sites, and (2) how complex topography influences on atmospheric conditions near emission sources impact plume concentrations at varying distances from the source. Two 133 Xe emission sources, including (1) a high flux rate of short duration representing an explosive event, and (2) a variable and continuous background source, are simulated. The continuous background source contributes significantly to total 133 Xe concentrations at several monitoring stations. Further, a WRF simulation at 9 km horizontal resolution is compared with a nested grid simulation, where the innermost domain has a resolution of 1 km. Increased topographic resolution leads to an improved representation of plume responses to local winds, with topographic influences greatest at locations closest to the sources. Differences between the two domain resolutions decrease at greater distances from the sources, as plumes have time to spread and mix and are influenced by synoptic scale circulation patterns that are represented similarly in both simulations.

54 ENVIRONMENTAL SCIENCES↗

Hanford Site Composite Analysis Special Analysis: P2R Model Predictive Contaminant Transport Simulations - Sensitivity Case

This environmental calculation file (ECF) documents the methodologies, assumptions, and results of predictive fate and transport simulations using the Plateau-to-River (P2R) model. This ECF supports the reevaluation of the representativeness of solid-waste radionuclide inventory and release rate from three solid waste sites included in the recently completed Hanford Site Composite Analysis (CA) (DOE-RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020)). Specifically, this ECF supports the reevaluation of the representativeness of the base case inventory and radionuclide waste release rates from three solid waste sites (i.e., 218-E-12B, 218-W-3A and 218-W-3AE) and two radionuclides (carbon-14 [C-14] and technetium [Tc-99]). These three waste sites and two radionuclides were identified as being the most significant contributors to groundwater contamination and dose in the CA at time periods after the compliance period. The release rates and footprints of the releases from the vadose zone are implemented in the fate and transport modeling utilizing the HSS package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tritium Transport Phenomena in Molten-Salt Reactors: Molten Salt Tritium Transport Experiment Design

Tritium is produced from neutron interactions with both lithium and beryllium. Large quantities of tritium are generated in Molten Salt Reactors (MSRs) which use LiF/BeF2 (FLiBe) as the fuel salt. Tritium is unique among the radionuclide hazards as it readily permeates through metal structural materials at high temperatures. All metal surfaces are potential release paths for tritium. For adequate safety analysis and eventual licensing of new reactors, predictive models for tritium transport and release from MSRs must be developed. These models must account for the multiple transport phenomena involved with tritium: fuel salt phase mass transport, dissociation/recombination reactions on metal surfaces, interstitial diffusion through the metal structure, and salt or gas phase mass transport in the downstream fluid. These models also must also be validated with representative experiments. Our previous report outlined tritium transport phenomena involved in MSRs, made suggestions on gaps in the transport dataset, and proposed an experimental test stand to test combined transport effects – tritium transport through pipe walls in a convective salt flow. In this report, we summarize an updated analysis framework for tritium transport in MSRs, report our results on hydrogen and deuterium permeation through Hastelloy N, and describe the final design of the Molten Salt Tritium Transport Experiment (MSTTE, pronounced “misty”). The MSRE provides the only wholistic experimental data set for tritium transport in MSRs and understanding the transport phenomena involved in the MSRE is crucial for future model development. One set of parameters in our analysis framework was unknown for the MSRE—surface reaction rates for tritium on Hastelloy N. This warranted our hydrogen and deuterium permeation campaign to assess the permeability, diffusivity, and solubility of hydrogen isotopes in clean Hastelloy N. Surface reaction rate constants were probed by low pressure measurements, however, no surface effects were observed in the limits of our permeation apparatus. Permeation experiments on oxidized Hastelloy N were not performed for this report but are planned in future work. The experimental test stand, MSTTE, measures combined transport properties of the salt-metal system. MSTTE is a forced convection FLiBe loop with custom designed test section to measure tritium transport through candidate structural materials. We use MSRE relevant dimensionless numbers to design and scale the test section. Hastelloy N is a candidate loop and test section material due to the relevance for the MSRE and related designs, however, other metals are being considered (e.g. 316H SS) which may better align with current vendor concepts.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Gas transport across the low-permeability containment zone of an underground nuclear explosion

Understanding the nature of gas transport from an underground nuclear explosion (UNE) is required for evaluating the ability to detect and interpret either on-site or atmospheric signatures of noble gas radionuclides resulting from the event. We performed a pressure and chemical tracer monitoring experiment at the site of an underground nuclear test that occurred in a tunnel in Nevada to evaluate the possible modes of gas transport to the surface. The site represents a very well-contained, low gaspermeability end member for past UNEs at the Nevada National Security Site. However, there is very strong evidence that gases detected at the surface during a period of low atmospheric pressure resulted from fractures of extremely small aperture that are essentially invisible. Our analyses also suggest that gases would have easily migrated to the top of the high-permeability collapse zone following the detonation minimizing the final distance required for migration along these narrow fractures to the surface. This indicates that on-site detection of gases emanating from such low-permeability sites is feasible while standoff detection of atmospheric plumes may also be possible at local distances for sufficiently high fracture densities. Finally, our results show that gas leakage into the atmosphere also occurred directly from the tunnel portal and should be monitored in future tunnel gas sampling experiments for the purpose of better understanding relative contributions to detection of radioxenon releases via both fracture network and tunnel transport.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Tracer Gas Model Development and Verification in PFLOTRAN

Tracer gases, whether they are chemical or isotopic in nature, are useful tools in examining the flow and transport of gaseous or volatile species in the underground. One application is using detection of short-lived argon and xenon radionuclides to monitor for underground nuclear explosions. However, even chemically inert species, such as the noble gases, have bene observed to exhibit non-conservative behavior when flowing through porous media containing certain materials, such as zeolites, due to gas adsorption processes. This report details the model developed, implemented, and tested in the open source and massively parallel subsurface flow and transport simulator PFLOTRAN for future use in modeling the transport of adsorbing tracer gases.

07 ISOTOPE AND RADIATION SOURCES↗

Real-Time Characterization of Salt Aerosols Generated from Static and Sparged Molten Salt

The formation of radionuclide-bearing aerosols in the respirable size range has the potential to significantly influence offsite dose consequences and is, therefore, an important consideration in nuclear facility safety assessments. Molten salt reactor (MSR) developers will likely need to demonstrate an understanding of the conditions under which radionuclide-bearing aerosols may be generated from their reactor under normal operating and accident conditions, as well as the characteristics and transport behavior of these aerosols, to demonstrate to the U.S. Nuclear Regulatory Commission (NRC) that the facility can be operated safely. Recent reviews of the literature identified a lack of experimental data describing the mechanisms of formation and properties (size, concentration, and composition) of salt aerosol particles that are produced from molten salts. Experiments that identify the conditions that lead to radionuclide-bearing salt aerosol releases and quantify the characteristics of salt aerosols formed by different mechanisms are high-priority needs to support MSR licensing. This report describes tests that were conducted within the Argonne Salt Aerosol Test Stand (a sealed vessel and measurement system) to generate salt aerosols from static and sparged molten salts and measure their size and concentration in real-time. The results provide insight into salt aerosol formation by the vapor condensation and bubble bursting mechanisms and inform the potential radiological consequences of aerosol formation from molten fuel salt. Videos of the salt surface were taken during salt sparge tests to observe surface bubble behavior. The data in this report can be used to develop mechanistic source term and accident progression models for MSRs. The real-time salt aerosol characterization technique used in this study will be employed in future integral effects tests that are conducted at an engineering scale to simulate realistic MSR accidents and in future separate effects tests to address additional variables that may impact salt aerosol characteristics (e.g., presence of fission products in salt and humidity in atmosphere).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗