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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Influences of Mg Ions and Al Ions on Deposition Behavior of Supersaturated Silicic Acid - 20261

Silicic acid can change into various species such as deposit, colloidal, and soluble form under certain conditions: for example, gradual pH changes around geological disposal repositories. In particular, silicic acid deposits narrow groundwater flow paths, thereby restricting the flow of groundwater. Such effects may contribute to a delay in radionuclide migration. Previous studies have reported that silicic acid supersaturated in sodium and calcium ions can narrow the flow paths. This study examined the effect of magnesium (Mg) and aluminum (Al) ions on the deposition of supersaturated silicic acid on the solid phase. The deposition behavior of supersaturated silicic acid on the solid phase was investigated in a batch system while changing the initial supersaturation concentration, the coexisting ion concentration, and the amount of added solid phase. In the presence of Mg ions, silicic acid precipitation increased with increasing Mg ion concentration due to the influence of the electrolyte, and crosslinking reactions. The coexistence of Al ions significantly suppressed silicic acid deposition due to the formation of a covering on the solid surface during Al ion hydrolysis under conditions of high Al concentration (1.4 mM). On the basis of these experimental results, the apparent deposition rate constant of silicic acid was estimated to be in the range from 10{sup -11} to 10{sup -10} m/s. The Damkoehler number (the dimensionless number expressed by the ratio of the characteristic time of mass transfer and the chemical reaction constant) was sufficient to cause the clogging of the host rock by deposition. This suggests that supersaturated silicic acid deposition, regardless of the presence of Mg ions (and Al ions), contributes to improving barrier performance against radionuclide migration in the host rock. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Lithologic controls on microfracturing from legacy underground nuclear explosions

Detection and verification of underground nuclear explosions (UNEs) can be improved with a better understanding of the nature and extent of explosion-induced damage in rock and the effect of this damage on radionuclide migration. Much of the previous work in this area has focused on centimeter- to meter-scale manifestations of damage, but to predict the effect of damage on permeability for radionuclide migration, observations at smaller scales are needed to determine deformation mechanisms. Based on studies of tectonic deformation in tuff, we expected that the heterogeneous tuff layers would manifest explosion-induced damage differently, with welded tuffs showing more fractures and nonwelded tuffs showing more deformation bands. In comparing post-UNE samples with lithologically matched pre-UNE equivalents, we observed damage in multiple lithologies of tuff through quantitative microfracture densities. We find that the texture (e.g., from deposition, welding, alteration, etc.) affects fracture densities, with stronger units fracturing more than weaker units. While we see no evidence of expected deformation bands in the nonwelded tuffs, we do observe, as expected, much larger microfracture densities at close range (<50 m) to the explosive source. We also observe a subtle increase in microfracture densities in post-UNE samples, relative to pre-UNE equivalents, in all lithologies and depths. The fractures that are interpreted to be UNE-induced are primarily transgranular and grain-boundary microfractures, with intragranular microfracture densities being largely similar to those of pre-UNE samples. This work has implications for models of explosion-induced damage and how that damage may affect flow pathways in the subsurface.

58 GEOSCIENCES↗
DOE OSTI2012

An Experimental Study of Diffusivity of Technetium-99 in Hanford Vadose Zone Sediments

One of the methods being considered at the Hanford site in Washington for safely disposing of low-level radioactive wastes (LLW) is to encase the waste in concrete and entomb the packages in the Hanford vadose zone sediments. The current plan for waste isolation consists of stacking low-level waste packages on a trench floor, surrounding the stacks with reinforced steel, and encasing these packages with concrete. Any failure of the concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. The mobilized radionuclides may escape from the encased concrete by mass flow and/or diffusion and move into the surrounding subsurface sediments. It is therefore necessary to conduct an assessment of the performance of the concrete encasement structure and the surrounding soil’s ability to retard radionuclide migration. The retardation factors for radionuclides contained in the waste packages can be determined from measurements of diffusion coefficients for these contaminants through concrete and fill material. Because of their anionic nature in aqueous solutions, the radionuclides, 99Tc and 129I were identified as long-term dose contributors in LLW. The leachability and/or diffusion of these radionuclide species must be measured in order to assess the long-term performance of waste grouts when contacted with vadose-zone porewater or groundwater. To measure the diffusivity, a set of experiments were conducted using 99Tc-spiked concrete (with 0 and 4% metallic iron additions) in contact with unsaturated soil half-cells that reflected the typical moisture contents of Hanford vadose zone sediments. The 99Tc diffusion profiles in the soil half cells were measured after a time lapse of ~1.9 yr. Using the concentration profiles, the 99Tc diffusivity coefficients were calculated based on Fick’s Second Law.

techetium, diffusion, vadose zone sediments↗
DOE OSTI2013

Colloid-Facilitated Radionuclide Transport in Fractured Carbonate Rock from Yucca Flat, Nevada National Security Site

In the Yucca Flat basin of the Nevada National Security Site (NNSS), ~750 nuclear detonations were conducted, primarily within the tuff confining unit (TCU) and the overlying alluvium. The regional carbonate aquifer (lower carbonate aquifer) is located below the TCU and is the most likely pathway for radionuclide migration off the NNSS. The regional carbonate aquifer underlies most of the NNSS and is known to be highly transmissive. Two principal pathways for LCA contamination exist in Yucca Flat. The first is composed of shortcuts (e.g. fractures) through the TCU which may provide a radionuclide transport pathway from tests conducted in the overlying alluvium and volcanics. The second is the release and migration of radionuclides from a small number (four) of tests conducted directly in the carbonate rock. Two of those tests were located near the saturated zone (Nash and Bourbon).

58 GEOSCIENCES↗
DOE OSTI2012

Strategy for Long-Term Stewardship and Monitoring of Amchitka Island - 12190

The Long-Term Surveillance and Maintenance Plan (LTSMP) for Amchitka details how the U.S. Department of Energy (DOE) intends to fulfill its mission to maintain protection of human health and the environment at and around the sites on Amchitka Island. The LTSMP calls for monitoring to be performed every 5 years, at least in the initial phase of the project. The purpose of the monitoring is to develop a baseline of activity concentrations for selected radionuclides in biota, water, and soil, both on Amchitka and at the reference location on Adak Island, approximately 322 km (200 miles) northeast of Amchitka. Data compiled by the Consortium for Risk Evaluation with Stakeholder Participation (CRESP, 2006) are being included as part of the baseline data set. The specific biological, water, and sediment samples collected during the 2011 sampling event were developed through close coordination with the primary stakeholders, including the Alaska Department of Environmental Conservation, the Aleutian Pribilof Island Association, and the U.S. Fish and Wildlife Service (USFWS). Amchitka is managed by the USFWS as part of the Alaska Maritime National Wildlife Refuge. Two plans were developed to address specific needs of the biological- and the terrestrial-monitoring programs. Results from these monitoring programs will help determine whether the environment is being impacted by radionuclide migration and uptake, and if subsistence and commercial-catch seafood is safe for human consumption. The RESRAD-BIOTA code is being used to evaluate ecological health relative to the radionuclide levels determined from this sampling event. The samples were sent to three laboratories for analysis. With the exception of the seawater samples, most of the samples were sent to the Center for Accelerator Mass Spectrometry at the Lawrence Livermore National Laboratory. A smaller subset of rock-weed samples, Star reindeer lichen samples, and soil samples collected from beneath the lichen were sent to UAF for cesium-137 analysis. Marine sediment samples were also collected and sent to UAF for testing. The seawater samples were sent to the University of Miami Tritium Laboratory for enriched tritium analysis. Results from the seawater samples for tritium were received in September 2011. Results from the 2011 sampling are expected to be available on the LM web site in 2012. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Disposing of waste package with respect to physico-chemical characteristics - 15041

The waste inventory to be taken into account for the design of the Cigeo project is defined in the industrial program for waste management established in cooperation between nuclear operators (EDF, AREVA, CEA) and Andra. This waste inventory has been constituted with a list of different families of radioactive waste packages from High Level Waste (HLW) to Intermediate Level Long-lived Waste (IL-LLW). IL-LLW include a large variety of items such as structural elements from fuel assemblies (cladding from the fuel rods called 'hulls', end pieces called 'end caps' and assembly spacer grids, etc.), sludge from effluent treatment or miscellaneous equipment (filters, pumps, etc.). Most ILLW (except solidified sludges) are basically metallic but organic and inorganic components such as plastics (cellulose, PVC...) and salts may also be included. The rules used for designing Cigeo are based on the separation of waste having different physico-chemical characteristics in different cells. However it could be possible to dispose of waste packages with different physico-chemical characteristics in the same cell if we can demonstrate that a type of waste does not generate significant physico-chemical perturbations on other co-stored families. The first step of our analysis has been the identification of categories of materials present in waste likely to interact with each other. The second step consisted in analysing qualitatively the physico-chemical interactions between these materials. In the third step, we defined criteria allowing evaluation of the consequences of these interactions on (i) gas production (mainly H{sub 2}), (ii) radionuclide release and transfer and (iii) degradation of concrete components of the disposal cell. We built then a table allowing qualitative comparison of the consequences of the interactions between the materials types defined in the first step. The conclusion of this study shows that it is necessary to pay a very careful attention before disposing of waste packages containing organic components nearby waste packages containing actinides radionuclides. The geochemical phenomena coupling must also be quantitatively evaluated so as to analyse possible interaction processes between the released organic compounds and the cementitious components of the cells, the near-field clay-stone and the radionuclides migration. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Leaching behaviour of low Ca:Si ratio CaO–SiO{sub 2}–H{sub 2}O systems

A dynamic leaching study of the dissolution of low calcium to silicon ratio (C/S) calcium–silicate–hydrate (C–S–H) systems with initial C/S ranging from 0.2 to 0.6 has been undertaken. Dissolution was studied in demineralised water at 25 °C to a degree of leaching of 2.5 m{sup 3} kg{sup −1}. These C–S–H gels show remarkably similar behaviour during early leaching stages, giving an equilibrated pH of ~ 9.9 and a solution phase C/S of ~ 0.29. Over longer times, C–S–H gels with C/S > 0.29 evolve, on leaching, towards a congruent dissolution point with a solid C/S close to 0.84 (consistent with tobermorite) and pH ~ 10.8. C–S–H gels with C/S < 0.29 become increasingly silica-rich on leaching but maintain an alkaline pH > 9.5 down to at least C/S = 0.07 (the lowest ratio reached). For C/S < 0.7, chemical modelling and X-ray diffraction data support an explanation of the incongruent dissolution behaviour of the low C/S C–S–H gels based on the congruent dissolution of distinct amorphous silica and tobermorite-like C–S–H phases. Above C/S of 0.7, the dissolution data are well described by an ideal solid solution model for the C–S–H phases. These results are of relevance to the consideration of the disposal of silica-rich vitrified intermediate-level radioactive wastes in cement-based concepts for geological disposal, where maintenance of alkaline pH values forms a key component of the chemical barrier to radionuclide migration. The implications are that the long-term pH buffering capacity provided by cementitious backfill materials would not be significantly affected by interactions with silica-rich wasteforms, which may lower the net C/S ratio of C–S–H phases, due to the natural tendency of these systems to restore congruent dissolution at pH 10.8.

36 MATERIALS SCIENCE↗
DOE OSTI2019

A Comparison of GoldSim, RESRAD-Onsite, and NORMALYSA Modeling Tools at Radioactive Waste Sites - 19480

Radioactive waste disposal and associated decision making is a challenging problem around the world. A strong performance assessment model plays a crucial role in making good management and remediation decisions and in optimizing the performance of a site. The International Atomic Energy Agency (IAEA) MODARIA II Working Group 1 (WG1) is comparing the performance of various modeling platforms used at Naturally Occurring Radioactive Material (NORM) and legacy waste sites to support risk-informed decision making. Neptune and Company, Inc. (Neptune) has developed probabilistic performance assessment models using the GoldSim system modeling software at a variety of radioactive waste sites. This paper presents a comparison between GoldSim and two other tools used to evaluate radiation exposure and their associated risks: the NORM And Legacy Site Assessment (NORMALYSA) tool used to assess risk at the Zapadnoe mill tailings site, and the residual radioactivity (RESRAD-Onsite) computer program used to calculate Authorized Limits at the Los Alamos National Laboratory (LANL). The International Atomic Energy Agency (IAEA) supported development of NORMALYSA based off of Ecolego 6.0, in which the user connects several universal modules, representing various environmental transport and exposure pathways, and enters in site-specific data. Further work with NORMALYSA has continued under the MODARIA II WG 1. A radionuclide transport and dose calculation model of the Zapadnoe uranium mill tailings site at the Pridneprovsky Chemical Plant in the Ukraine has been configured by MODARIA II WG1 to test the capabilities of NORMALYSA. Under this test case, contaminant transport and effective dose calculations were performed for two exposure scenarios. The onsite worker is exposed via external ground irradiation and radon and radioactive dust inhalation. The offsite resident defines a residence established 300 years after institutional control has ended, 800 meters downstream from the site with exposure pathways including: ingestion of garden vegetables irrigated by contaminated ground water, ingestion of fish from the Konoplyanka River and agricultural activities in the contaminated garden. GoldSim modeling software is a dynamic probabilistic modeling platform that evaluates uncertainty in a robust and transparent manner. Although GoldSim provides contaminant and radionuclide transport modules to facilitate integrated modeling of radionuclide migration in the environment, these features are not embedded in an existing modeling framework, except as created by the user. Neptune developed a GoldSim model for the two exposure scenarios of the Zapadnoe test case. Neptune's Generic PA Model was used as a starting point for the Zapadnoe site. Input parameters for the GoldSim model include site-specific parameters from the MODARIA Working Group as well as parameters from the Generic PA Model and other PA models created by Neptune. For the other comparison, Version 7.0 of RESRAD-Onsite, developed by Argonne National Laboratory for the U.S. Department of Energy (DOE), was used to calculate Authorized Limits for LANL. Authorized Limits are concentrations of radionuclides in soil that support the evaluation process to clear land for release under different uses. The RESRAD-Onsite computer code was used to calculate Authorized Limits because this program was specifically designed to derive radionuclide soil guidelines corresponding to a specific dose criterion. The scope of the RESRAD dose or risk evaluation is constrained to the transport and exposure pathways that have been included in the computer code. To assist in illustrating the capability of GoldSim modeling software, a GoldSim model was created to replicate the calculation of LANL's Authorized Limits for soil. The main exposure pathways in this model are inhalation of dust and gas, plant ingestion, soil ingestion, and external ground irradiation. All of the processes and outputs of RESRAD-Onsite and NORMALYSA can be created in a GoldSim model, but the value of GoldSim lies in its flexibility for application to any of a wide variety of environmental modeling problems. GoldSim allows development of site-specific inventory, transport mechanisms and risk assessment scenarios. If all potentially complete release, transport, and exposure pathways are addressed in an existing dose and risk assessment computer code, and if the code's capabilities fulfill the project modeling objectives, then expending resources to create a GoldSim model may not be necessary. Site optimization and good decision making about site management are often best when supported with the flexibility of GoldSim as a modeling tool. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

A consistent approach for the development of a comprehensive data base of time-dependent parameters for concrete engineered barriers

This paper presents a consistent approach for the development of a comprehensive data base of time-dependent hydraulic and transport parameters for concrete engineered barriers of the future Dessel near surface repository for low level waste. The parameter derivation is based on integration of selected data obtained through an extensive literature review, data from experimental studies on cementitious materials specific for the Dessel repository and numerical modelling using physically-based models of water and mass transport. Best estimate parameter values for assessment calculations are derived, together with source and expert range and their probability density function wherever the data was sufficient. We further discuss a numerical method for up-scaling laboratory derived parameter values to the repository scale; the resulting large-scale effective parameters are commensurate with numerical grids used in models for radionuclide migration. To accommodate different levels of conservatism in the various assessment calculations defined by ONDRAF/NIRAS, several sets of parameter values have been derived based on assumptions that introduce different degrees of conservatism. For pertinent parameters, the time evolution of such properties due to the long-term concrete degradation is also addressed. The implementation of the consistent approach is demonstrated by considering the pore water diffusion coefficient as an example. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Numerical Techniques for Radioactive Waste Repository Safety Assessment Based on Transport in Geological Media Models - 12083

Radionuclide migration in geological media is considered within the framework of safety assessment of radioactive waste disposal facility. In this context groundwater flow and transport models are necessary. Computational technologies allowing for semiautomatic generation of unstructured meshes with different cell types, i.e. tetrahedra, hexahedra and pyramids and the subsequent solution of groundwater flow problems on these meshes are introduced. The application of methods is demonstrated in the groundwater flow model for a decommissioned subsurface reactor vessel, buried on its current location. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Uncertainty quantification of a radionuclide release model using an adaptive spectral technique

In this paper we present the application of a non-intrusive spectral techniques we recently developed for the evaluation of the uncertainties associated with a radionuclide migration problem. Spectral techniques can be used to reconstruct stochastic quantities of interest by means of a Fourier-like expansion. Their application to uncertainty propagation problems can be performed by evaluating a set of realizations which are chosen adaptively, in this work the main details about how this is done are presented. The uncertainty quantification problem we are going to deal with was first solved in a recent work where the authors used a spectral technique based on an intrusive approach. In this paper we are going to reproduce the results of this reference work, compare them and discuss the main numerical aspects. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Post-Closure Environmental Sampling and Inspection at the Amchitka Island, Alaska, Site - 17251

In the 1960's and early 1970's, three underground nuclear tests were conducted on Amchitka Island, Alaska. In 1965, the US Department of Defense-in conjunction with the US Atomic Energy Commission (AEC)-conducted the first of these nuclear tests, Long Shot, to provide data that would improve US capabilities for detecting underground nuclear explosions. In 1969, AEC conducted the second test, Milrow, to explore the feasibility of detonating a much larger device. In 1971, AEC conducted the third test, Cannikin, which was the largest underground test ever conducted by the US. The Long-Term Surveillance Plan (LTSP) for the Amchitka, Alaska, Site details how the US Department of Energy Office of Legacy Management (LM) intends to fulfill its mission to protect human health and the environment at and around the Amchitka Island site. The LTSP calls for monitoring to be performed every 5 years, at least during the initial phase of the project. The purpose of the monitoring is to develop a baseline of activity concentrations for selected radionuclides in biota, water, and soil, both on Amchitka Island and at the reference location on Adak Island, approximately 322 kilometers (200 miles) northeast of Amchitka. In addition to the environmental monitoring activities, seven mud pit caps that contain diesel-contaminated soils are inspected. The plan for biological and water sampling (both seawater and freshwater) during the May 2016 sampling event was developed through close coordination with the primary stakeholders, including the Alaska Department of Environmental Conservation, the Aleutian Pribilof Islands Association, and the US Fish and Wildlife Service. The environmental sampling in 2016 is a continuation of LM's evaluation of Amchitka Island's environment. Previous results from similar monitoring programs in 2004 and 2011 indicate that the environment is not being impacted by radionuclide migration and uptake from the underground nuclear testing conducted beneath Amchitka Island; consequently, subsistence and commercial-catch seafood is safe for human consumption. The collection of biota samples (rockfish, Irish lords, greenling, and rockweed) for cesium-134 ({sup 134}Cs), cesium-137 ({sup 137}Cs), plutonium-239 ({sup 239}Pu), plutonium-240 ({sup 240}Pu), and freshwater and seawater samples for {sup 134}Cs, {sup 137}Cs, and tritium ({sup 3}H) was the primary objective of the 2016 sampling effort. Rockfish, Irish lords, and greenling are resident, nonmigratory fish species that spend their entire life cycle in the marine environment, and rockweed is an inter-tidal species that may concentrate cesium. The seawater samples were collected primarily to determine if leakage from the Long Shot detonation could be detected and, secondarily, to compare with the background seawater samples collected from Adak Island. Cesium isotopes are also being analyzed to better understand the potential impact that the Fukushima-Daiichi release might have on the Amchitka and Adak environments. The target detection limits used for the 2016 sampling are lower than those used in previous studies. The lower detection limits make it possible for LM to delineate background activity levels for the radionuclides of interest. Data from the 2016 sampling event go beyond assessing food safety and focus on detecting leakage from the underground nuclear explosions. Additionally, the baseline activity concentrations obtained for the reference area (Adak Island) will enable identification of quantitative statistical trends in the results of future sampling programs. Sampling programs conducted in 2021 and beyond will have an objective to assess the statistical trends of radioactivity levels in the Amchitka Island environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

The fourth decade of underground research at the Grimsel Test Site - what we have learned and where we go from here - 15075

At the Grimsel Test Site, NAGRA and its partners have celebrated thirty years' worth of essential contributions to the characterization of crystalline host rock, and the development and confirmation of safe geological disposal concepts. In operation since 1984, the underground research laboratory in the Swiss Alps shall not accept radioactive waste but can host experiments with radiotracers/radionuclides under strictly controlled conditions. The strong drive for international cooperation at the Grimsel Test Site is reflected in the more than two dozen organizations and research institutes from twelve countries and the European Union which have participated in the research program to date. The program has been designed dynamically to always mirror the current requirements of national programs for the long-term management of radioactive waste, as well as attempt to anticipate the next steps. Early work featured the development of methodologies for formation characterization. Then followed a period concentrating on performance assessment issues, before radionuclide migration and barriers were investigated intensely. The past 15 years have been dominated by engineering demonstration experiments. The research conducted at the Grimsel Test Site has complemented laboratory experiments, surface investigations and numerical modelling studies through the bridging of different scales and drawing off links between laboratory setups and natural analogues. The crystalline rock formations of the Aar Massif have provided an opportunity to do experiments in environments similar to those of future repositories. The facility also serves as a platform for continual knowledge transfer between generations of scientists and fosters synergies among disciplines. However, considering the ambitious schedule for repository implementation in several continuous, one may ask whether the era of generic underground rock laboratories is approaching its end. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Optimising National WM Strategies through early consideration of Nuclear Safeguards - 18607

International Atomic Energy Agency (IAEA) safeguards stand alongside safety and security as one of the three pillars for prudent management of all nuclear material, including nuclear waste. Although safety considerations, including public and environmental radiation protection, are the traditional drivers of waste management strategies, there is a requirement for nuclear safeguards in shaping and quantifying long-term solutions for special classes of radioactive waste. This is especially important when considering the disposal of nuclear material in a repository that could be released from regulatory oversight for radiation protection after a period of institutional control, as some safeguards oversight would still be required. Failure to consider nuclear safeguards at the early stages of planning may alternatively lead to excessive volumes for disposal or the need to recondition already treated wastes. At the very least, safeguards measures should be considered before countries seek to dispose of legacy nuclear materials, decommissioning wastes and other materials containing uranium, thorium or plutonium in an operating repository. Nuclear safeguards are the set of tools and techniques used by the IAEA to verify that countries comply with their international obligations not to divert nuclear materials to nuclear explosive devices. Under the Nuclear Non-Proliferation Treaty (NPT), nuclear safeguards apply to all uranium, thorium and plutonium held in non-weapons NPT states, with limited exceptions. In nuclear-weapon states, much of their material is likewise subject to IAEA safeguards through conditions in agreements with respective suppliers of the uranium. Under IAEA safeguards, such nuclear material must remain accounted for and accessible for periodic verification-analogous to the safety concepts of reversibility and retrievability. Nevertheless, safeguards requirements can be terminated - provided that the State and the [IAEA] agree that such nuclear material is practicably irrecoverable - through dilution or immobilisation in solid form (such as cement, glass or ceramic). This means candidate material can be disposed of as non- nuclear material, with no further safeguards requirements, provided this criterion is met. Unlike radiological wastes where repository design strongly influences pathways for radionuclide migration and overall safety performance, repository design is not a factor in considering the termination of safeguards on nuclear material. This paper looks at similarities and differences in the safety, security and safeguards regulatory requirements for the management of radioactive waste and nuclear material in Australia. In particular, it outlines recent experience gained from participation in Australia's waste acceptance criteria working group for a national low-level waste repository and intermediate-level waste store, as well as from Australia's overall waste management strategy. These items of work have coincided with the IAEA update of its internal policy on termination of safeguards on nuclear material. Australia's experience shows how inclusion of safeguards criteria in the planning process is leading to optimisations in choice of facility concepts, project sequencing and equitable distribution of economic risk. By considering the three pillars-safety, security and safeguards-early on in the planning process, Australia's waste management strategy will provide a benchmark for other states in establishing and updating their own waste acceptance criteria for the disposal of nuclear material. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Assessment of Tritium Activities in Bailed versus Pumped Samples from Wells at the Nevada National Security Site

The Underground Test Area (UGTA) Activity uses a variety of methods to collect groundwater samples to identify radionuclide migration from underground nuclear tests. These include depth-discrete bailing, pumping with low-volume rod pumps, and pumping with electrical submersible pumps. The Nevada National Security Site (NNSS) Integrated Groundwater Sampling Plan specifies that when sampling with a pump, a minimum of three effective well volumes are withdrawn and then samples are collected after water-quality parameters have stabilized. In locations where pumping is not feasible, depth-discrete bailing is used and purging prior to sampling is usually not required. A recent study evaluated three sampling technologies and recommended that historical tritium results be evaluated where both pumped and bailed samples are available to identify preferred sampling protocols for the collection of tritium samples. The tritium ( 3 H) activities were obtained from the UGTA chemistry data base. Wells were identified with known 3 H activities above method detection limits, and then evaluated if both bailed and pumped samples had been collected. Twenty two wells and piezometers with bailed samples, pumped samples, and 3 H activities above background were identified for further consideration. The conclusions from this analysis are: Bailed samples collected for 3 H analysis near the water surface in a well are lower in 3 H activity than bailed samples from within screened intervals and pumped samples. Depth-discrete bailed samples from within the screened intervals are generally in good agreement with pumped samples from developed wells and piezometers. Depth-discrete bailed samples from undeveloped wells and piezometers are in good agreement with the first pumped samples. However, the next pumped samples increased in 3 H activity, resulting in a greater percent difference between the undeveloped bailed samples and later pumped samples. Continuous pumping over extended periods removing large purge volumes from wells can perturbate the surrounding groundwater system for long periods of time. These perturbations can cause large changes in 3 H activities in the aquifer near the well because of the mixing of groundwater with variable 3 H activities. Recommendations include: Bailed samples for 3 H should not be collected near the water surface in the well. Bailed samples should be collected from within the well screen. Logs of temperature, chemistry, and thermal flow should be evaluated to identify optimal depths within the well screen to collect depth-discrete bailer samples. Purging of large volumes of water from the well over extended periods of time should be avoided when collecting 3 H samples. Sufficient time should be allowed after pumping large volumes of water from the well (e.g., after well development) for the surrounding aquifer and 3 H activities to return to ambient conditions

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Potential applications of microbial genomics in nuclear non-proliferation

As nuclear technology evolves in response to increased demand for diversification and decarbonization of the energy sector, new and innovative approaches are needed to effectively identify and deter the proliferation of nuclear arms, while ensuring safe development of global nuclear energy resources. Preventing the use of nuclear material and technology for unsanctioned development of nuclear weapons has been a long-standing challenge for the International Atomic Energy Agency and signatories of the Treaty on the Non-Proliferation of Nuclear Weapons. Environmental swipe sampling has proven to be an effective technique for characterizing clandestine proliferation activities within and around known locations of nuclear facilities and sites. However, limited tools and techniques exist for detecting nuclear proliferation in unknown locations beyond the boundaries of declared nuclear fuel cycle facilities, representing a critical gap in non-proliferation safeguards. Microbiomes, defined as “characteristic communities of microorganisms” found in specific habitats with distinct physical and chemical properties, can provide valuable information about the conditions and activities occurring in the surrounding environment. Microorganisms are known to inhabit radionuclide-contaminated sites, spent nuclear fuel storage pools, and cooling systems of water-cooled nuclear reactors, where they can cause radionuclide migration and corrosion of critical structures. Microbial transformation of radionuclides is a well-established process that has been documented in numerous field and laboratory studies. These studies helped to identify key bacterial taxa and microbially-mediated processes that directly and indirectly control the transformation, mobility, and fate of radionuclides in the environment. Expanding on this work, other studies have used microbial genomics integrated with machine learning models to successfully monitor and predict the occurrence of heavy metals, radionuclides, and other process wastes in the environment, indicating the potential role of nuclear activities in shaping microbial community structure and function. Results of this previous body of work suggest fundamental geochemical-microbial interactions occurring at nuclear fuel cycle facilities could give rise to microbiomes that are characteristic of nuclear activities. These microbiomes could provide valuable information for monitoring nuclear fuel cycle facilities, planning environmental sampling campaigns, and developing biosensor technology for the detection of undisclosed fuel cycle activities and proliferation concerns.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2016

Deposition Behavior of Supersaturated Silicic Acid on Ca-type Bentonite in Geological Disposal System - 16033

For backfilling tunnels in geological disposal systems, the degradation of the low permeability of Na-type bentonite by ion-exchanging to Ca-type is a concern. The deposition of silicic acid around a repository with the dramatic change in pH due to the use of cement causes the clogging of the flow-path and pore space. Such effect may contribute to a more effective barrier performance for radionuclide migration in the backfill. As a first step to clarifying the clogging effect in the backfill, this study examined the deposition of supersaturated silicic acid on Ca-type bentonite. In the deposition experiments, the supersaturated silicic acid solution (250 ml, 4-10 mM, pH>10) was poured into a polyethylene vessel containing Ca-type bentonite (2.5-10.0 g). The deposition of silicic acid was started by setting the pH to 8. As a result, supersaturated silicic acid significantly deposited on Ca-type bentonite under all experimental conditions of supersaturated silicic acid concentration. The experimental results showed that the deposition rate-constants were in the order of 10-11 m/s. Our previous study showed the clogging effect in rocks by using numerical simulation with the same order rate-constants. These findings suggest that the deposition of supersaturated silicic acid on Ca-type bentonite causes the retention of low permeability and the retardation effect for radionuclides by the clogging effect in backfilled tunnels. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Radionuclide Waste Disposal: Development of Multi-scale Experimental and Modeling Capabilities (Final Report)

The DOE EPSCoR Implementation project “Radioactive waste management: Development of multi-scale experimental and modeling capabilities” helped to develop a team of scientists and engineers from Clemson University, South Carolina State University, and the University of South Carolina to address the disposition of nuclear wastes and study the transport of radioisotopes from a waste repository in the near and far field. The project involved 20 faculty from the three institutions as well as 13 postdoctoral fellows, 32 graduate students, and 32 undergraduate students and was active from 2014-2019. Additionally, we forged new collaborations with nine researchers from DOE laboratories SRNL, LLNL, and ANL as well as the University of Manchester and the China Academy of Engineering Physics. The overarching goal of the project was to understand the conditions under which important classes of co-reactants, ranging from counter ions in crystal lattices to dissolved oxygen in pores, control the chemistry and transport characteristics of radionuclides in engineered waste forms and natural soils. Our approach was to characterize the time and length scales over which non-equilibrium states are maintained by rate-limiting, or rate-enhancing, reactions between radionuclides and co-reactants due to interactions between physical mass-transfer processes (i.e., advection, diffusion) and (biogeo) chemical reactions. We have focused our project on three specific classes of reactions relevant to radionuclide transport at DOE legacy sites: ion exchange/substitution, ligand complexation, and redox-mediated reactions. Understanding radionuclide migration requires detailed knowledge of how changes to a system – whether engineered or natural – drive the behavior of co-reactants, which in turn provide the geochemical context controlling radionuclide transport. Student engagement and training were a primary focus of the project in order to create a pipeline of researchers who could work in the area of nuclear waste disposition to support the state and the nation. Over the duration of the project we worked with 32 undergraduate, graduated 18 M.S. students and 14 Ph.D. students, and advised 13 postdoctoral fellows. The Ph.D students and postdocs have primarily taken positions at DOE laboratories, academia, and industry. Through our collaborative team, numerous follow on projects have been started with over $5M in sponsored research. Additionally, thus far the team has published 53 peer reviewed papers and given over 75 technical presentations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗