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All sources NASA NTRS DOE OSTI

DOE OSTI2023

Examining the potential for detecting simultaneous noble gas and aerosol samples in the international monitoring system radionuclide network

The purpose of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) is to establish a legally binding ban on nuclear weapon test explosions or any other nuclear explosions. The Preparatory Commission for the CTBT Organization (CTBTO PrepCom) is developing the International Monitoring System (IMS) that includes a global network of 80 stations to monitor for airborne radionuclides upon entry into force of the CTBT. All 80 radionuclide stations will monitor for particulate radionuclides and at least half of the stations will monitor for radioxenon. The airborne radionuclide monitoring is an important verification technology both for the detection of a radionuclide release and in the determination of whether the release event originates from a nuclear explosion as opposed to an industrial use of nuclear materials. Nuclear power plants and many medical isotope production facilities release radioxenon into the atmosphere. Low levels of a few particulate isotopes, such as iodine, may also be released. Detections of multiple isotopes are useful for screening the radionuclide samples for relevance to the Treaty. This paper examines the anticipated joint detections in the IMS of noble gas and particulate isotopes from underground nuclear explosions where breaches in the underground containment vents from low levels to up to 1% of the radionuclide inventory of the resulting fission products to the atmosphere. Detection probabilities are based on 844 simulated release events spaced out at 17 release locations and one year in time. Six different release (venting) scenarios, including two fractionated scenarios, were analyzed. When ranked by detection probability, 11 particulate isotopes and one noble gas isotope ( 133 Xe) appear in the top 20 isotopes for all six release scenarios. Using the 11 particulate isotopes and the one noble gas isotope, the IMS has nearly the same detection probability as when 45 particulate and 4 noble gas isotopes are used. Thus, a limited list of relevant radionuclides may be sufficient for treaty verification purposes. The probability that at least one particulate and at least one radioxenon isotope would be detected in the IMS from the release events ranged from 0.15 to 0.86 depending on the release scenario.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2025

Computational Optimization of 133m Xe Production via Neutron Irradiation in a TRIGA Reactor

Here, the Comprehensive Nuclear-Test-Ban Treaty bans all nuclear tests worldwide. As part of treaty compliance, the concentration of radioactive nuclides in the atmosphere is monitored to detect nuclear weapons tests. Radioactive noble gas fission products, specifically radioxenon, can vent into the atmosphere after a nuclear weapons test, even if the test is well contained underground or underwater. Radioxenon thus serves as a signal for nuclear weapons tests. All atmospheric monitoring systems require samples of radioxenon isotopes for detector calibration, quality control, and certification. Here, we present a novel, improved method for creating samples of 133m Xe via neutron irradiation of 132 Xe in the Washington State University TRIGA reactor. 132 Xe neutron absorption results in either 133 Xe or 133m Xe—thermal neutron absorption results in 133m Xe 12% of the time, while fast neutron absorption (above ~1 MeV) results in 133m Xe ~50% of the time. To optimize the production of 133m Xe via neutron absorption in 132 Xe in the thermal TRIGA reactor, spectral tuning using an irradiation chamber is required to maximize the fraction of fast neutrons being absorbed and minimize the number of thermal neutrons interacting with the 132 Xe. We used MCNP to tally 132 Xe absorptions with the isotopic tally function, flux tallies and neutron attenuation to estimate the number of neutrons reaching the 132 Xe through the irradiation chamber, and the adjoint importance function to improve the source strength estimate. Additionally, we performed a heat transfer analysis for safety considerations. It was determined that the use of a 96% enriched 10 B boron carbide chamber, placed next to the fuel elements in reactor position D8, increases the 133m Xe/ 133 Xe activity ratio from a baseline value of 0.3 to 1.0, a 233% increase. Additionally, it was determined that the alpha heating produced in the boron does not become an unmanageable problem in the Washington State University reactor.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

DOE OSTI2023

Evaluation of Desiccation Behavior in Basalt Microfiber–Reinforced Bentonite Clay for Geological Repositories of Nuclear Spent Fuel Using Digital Image Correlation

ABSTRACT Secure storage of nuclear spent fuel (NSF) is of great concern for protecting public health and safety. The preferred long-term solution is underground containment in geological repositories, where one or more engineered barrier materials (EBM) encapsulate the NSF and separate it from the natural rock. Bentonite clay is commonly used as an EBM due to its many advantageous properties including low hydraulic conductivity, which ensures limitation of water infiltration to the system and the subsequent risk of corrosion in NSF canisters. However, bentonite clay subjected to heating from nuclear decay may form desiccation cracking. This study conducted disk-shaped free shrinkage tests and ring-shaped restrained shrinkage tests of bentonite clay samples reinforced with basalt microfibers. Digital image correlation was used as a noncontact full-field displacement measurement to track the time-evolving shrinkage and desiccation cracking phenomena and make quantified comparisons between plain bentonite and bentonite with varying contents of basalt microfibers (i.e., 0.0, 0.5, 1.0, and 1.5 % wt.). Results indicate that plain bentonite and basalt microfiber-reinforced samples showed similar free shrinkage behavior, while desiccation cracking behavior was significantly altered by adding basalt microfibers. Microfiber reinforcement effectively reduced major cracks through a “crack-bridging” effect while causing minor cracks to initiate earlier and at higher moisture contents than plain bentonite. Results infer that reinforcing plain bentonite with inorganic microfibers can potentially control desiccation cracking, leading to safer and improved nuclear waste management.

Materials Science↗

DOE OSTI2023

A study of explosive-induced fracture in polymethyl methacrylate (PMMA)

The fracture response of geologic materials is of interest for applications, including geothermal energy harnessing and containment of underground explosions. To better understand the explosively induced fracture response of geomaterials, polymethyl methacrylate (PMMA) was used as a transparent rock surrogate to allow imaging of internal shock propagation and fracture growth processes. Experiments were conducted using high-speed shadowgraphy and photon Doppler velocimetry (PDV), which were compared to numerical simulations. Experiments measured fractures produced in 304.8mm × 304.8mm × 304.8mm PMMA cubes with two simultaneously initiated detonators. The cubes were subjected to varying amounts and directions of externally applied uniaxial stresses, including no stress, 2 MPa stress, and 20 MPa stress. The fracture radius as a function of time was extracted from the high-speed videos. Post-test images of the PMMA cubes aided in the determination of three-dimensional effects not directly imaged by the cameras. The surface velocity history and the shock response captured in PDV and the high-speed videos were compared to the simulated explosive-induced shock response. The simulation results indicate that the shock drives the fracture for the first 20 μs corresponding to a fracture radius of approximately 15 mm in the experiments. The gas-driven fracture extent was estimated analytically using an equilibrium stress distribution calculated after the shock wave propagation through the sample. Reduction in the gas pressure due to the leakage of the explosive products through the crack as a function of time was accounted for. In conclusion, the estimated fracture lengths were in agreement with the experimentally observed fracture lengths.

15 GEOTHERMAL ENERGY↗

DOE OSTI2023

Low-Radioactivity Argon for Rare-Event Searches

39Ar and 42Ar produce irreducible backgrounds for several argon-based dark matter and neutrino experiments. The use of low-radioactivity underground argon (UAr) could be a solution to the problem. The DarkSide-50 experiment demonstrated that argon derived from underground sources can contain a much lower concentration of 39Ar than atmospheric argon. Following this success, the Global Argon Dark Matter Collaboration (GADMC) is procuring hundreds of tons of UAr for the DarkSide-20k detector. To serve the broader community need, it is increasingly important to identify new sources of low-radioactivity argon. In addition, understanding the underground production mechanisms of argon radioisotopes and devising methods to measure them at ultra-low levels is necessary. The use of low-radioactivity argon could be crucial to expanding the physics goals and sensitivity of next-generation large-scale argon-based experiments.

Radioargon isotopes, Underground argon, Isotope pr↗

DOE OSTI2025

Improved Fundamental Understanding of Aluminum Chemistry and Interactions of Aluminate Anion with Co-Anions: ORNL Project Progress Report

The U.S. Department of Energy (DOE)’s Hanford Site in Washington State houses 177 underground storage tanks containing millions of gallons of nuclear and chemical waste with high aluminum content. Aluminum (Al) salt reactions with strong bases produce aluminum hydroxides, like boehmite (γ-AlOOH), which are main components of insoluble nuclear waste sludge. Understanding the morphology, crystallinity, and dissolution behavior of boehmite under waste tank conditions is necessary for improving waste management and mitigation strategies. The ORNL team uses in situ multimodal analysis strategy to study Al chemistry of simulated tank waste using microfluidic reactors and advanced chemical imaging and mass spectrometry (MS) techniques. Because the SALVI device is vacuum compatible and transferrable among different platforms, we can use it in scanning electron microscopy (SEM), vacuum ultraviolet single photon mass spectrometry (VUV SPI-MS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) to study the chemical speciation and colloid stability in liquids in this project. Additionally, ex situ transmission electron microscopy (TEM) and x-ray diffraction (XRD) spectroscopy can be used to verify particle phase to further the understanding of the Al-bearing phases. This report gives a summary of the technical progress of the ORNL tasks. A plan for year 2 performance is recommended in the summary.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Detection and Association of Operational Events using DAS and Seismometers (FY 2025 Mid-Year Report)

This mid-year report summarizes ongoing work to identify anomalous vibration signals indicative of potential containment breaches. This work includes compiling continuous seismic datasets and testing and refining underground detection and geolocation techniques. In the first two quarters of FY25, we have completed two project work plan tasks: (1) creating a database of continuous waveforms and ground truth event data from multiple modalities and (2) refining and implementing a detection and association algorithm to create a catalog of anomalous underground activities. This report contains a summary of the seismic database including the continuous seismic data collected by a dense array of surface seismic stations above Pleasant Gap Mine, and continuous seismic data collected using subsurface distributed acoustic sensing (DAS) in the subsurface at Sanford Underground Research Facility (SURF) and the ground truth information gathered from both sites. This report also includes results from refining and applying a dynamic power spectral density detector to both continuous seismic datasets. Finally, the report provides an initial catalog of subsurface operational events from both sensing modalities.

58 GEOSCIENCES↗

DOE OSTI2023

Simulations of Criticality Control Overpack Container Compaction at the Waste Isolation Pilot Plant

Criticality Control Overpack (CCO) containers are being considered for the disposal of defense-related nuclear waste at the Waste Isolation Pilot Plant (WIPP). At WIPP, these containers would be placed in underground disposal rooms, which will naturally close and compact the containers closer to one another over several centuries. This report details simulations to predict the final container configuration as an input to nuclear criticality assessments. Each container was discretely modeled, including the plywood and stainless steel pipe inside the 55-gallon drum, in order to capture its complex mechanical behavior. Although these high-fidelity simulations were computationally intensive, several different material models were considered in an attempt to reasonably bound the horizontal and vertical compaction percentages. When exceptionally strong materials were used for the containers, the horizontal and vertical closure respectively stabilized at 43:9 % and 93:7 %. At the other extreme, when the containers completely degraded and the clay seams between the salt layers were glued, the horizontal and vertical closure reached respective final values of 48:6 % and 100 %.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

FY25 Task 5: Small-Scale Mixing

The U.S. Department of Energy (DOE) Hanford Site has 177 underground storage tanks that contain a complex and diverse mix of chemical and radioactive wastes from past nuclear fuel reprocessing and waste management operations. The strategy of the DOE Hanford Field Office is to retrieve this waste, ~20 vol% of which is in the form of insoluble undissolved solids (UDS) or sludge, and treat it via immobilization at the Hanford Waste Treatment and Immobilization Plant (WTP). The diverse properties and characteristics of Hanford tank waste lead to major challenges related to its transport from the underground tanks to the WTP. These challenges, however, can be addressed by investigating the behavior of tank waste samples and simulant materials and evaluating their behavior against the capabilities of mixing and transport system designs that may be incorporated to retrieve and treat the waste.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Identification of SPR Caverns with Multiple Oil Layers

This analysis shows that when lower density crude oil is injected into the top of an underground salt storage cavern containing more dense crude, separate oil phases can form and coexist indefinitely. This has been observed at the U.S. Strategic Petroleum Reserve in spite of geothermal heating and natural convection, which tend to mix the contents of containers with significant vertical extent subjected to wall and bottom heating. Such persistent layering can create operational challenges for meeting delivery specifications if high-value, low-vapor pressure oil becomes trapped below incoming low-density, high-vapor pressure oil, effectively blocking access to the lower layers until the top layer is removed. Previous conceptual models assumed that the oil injection process mixed incoming oil with resident oil in a storage cavern, forming a single oil phase with relatively homogeneous properties. Here, a review of historical data from the Strategic Petroleum Reserve revealed that several caverns contain multiple oil layers. As a result, oil layering needs to be another variable considered when planning oil movements at SPR in order to optimize low-vapor pressure oil availability to assist in oil delivery blending.

02 PETROLEUM↗

DOE OSTI2022

Sludge Processing Options for early HLW Treatment at Hanford

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Evaluation of High Level Waste Sludge Processing Behavior

The U.S. Department of Energy’s (DOE) Hanford Site has 177 underground storage tanks that contain wastes from past nuclear fuel reprocessing and waste-management operations. Over 20% of this waste is in the form of an insoluble sludge that will require slurry modification before its transfer to the Waste Treatment and Immobilization Plant (WTP). Specific WTP acceptance criteria for waste feed delivery describe the physical and chemical characteristics of the waste that must be met before the waste is transferred to the WTP. One challenging requirement relates to the undissolved solids (UDS) composition in a waste feed because the waste contains solid particles that settle, and their concentration and relative proportion can change during the transfer of the waste in individual batches. A key uncertainty is the ability to transfer and mix wastes with large variations in UDS concentrations and resulting settling rates. To address this uncertainty, a number of small scale mixing and settling tests have been conducted to determine the mobilization performance of variable chemistry simulants. Comparison of the size and density of the particulate for each simulant to that of southeast area Hanford sludge was made using metrics for particle mobilization, suspension, settling, and pipeline transfer where dependance on particle size and density may be different, including: 1. Settling velocity, 2. Critical shear stress for erosion, 3. Just-suspended impeller speed, and 4. Pipeline critical transport velocity. Existing high-level waste sludge data has shown the effect that increasing Al concentration has on resulting settled solids. This differential settling of particles in the sludge has the possibility of resulting in solids segregation during feed preparation and uneven particle distribution during pipeline transportation or mixer jet pump operations. Understanding the predictive capabilities of HLW solids settling and transport as well as potential remedies for addressing disparate sludge behaviors can help provide technical guidance during HLW flowsheet planning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

The Low-Yield Nuclear Monitoring (LYNM) Experimental Science Plan

The Low-Yield Nuclear Monitoring (LYNM) Program is a long-term NNSA research and development effort designed to improve the United States’ explosion monitoring capabilities, particularly with respect to low-yield and potentially evasive underground nuclear testing. The LYNM Program focuses on researching, discovering, and exploiting unique and useful signatures, from all available technologies and sensors (e.g., seismic, acoustic, electromagnetic, gases, and particulates (both stable and radioactive)). Four Department of Energy laboratories participate in LYNM and together are referred to as the ‘quad-lab’. The R&D program execution is performed under NNSA defined structures known as “ventures”. Four science ventures were established: 1) Explosion Source Functions; 2) Containment of Low-Yield Underground Tests; 3) Local Signatures; 4) Dynamic Monitoring Networks. To organize and execute the large field scale experiment a fifth venture was established: 5) Physics Experiment One (PE-1). As part of the LYNM Program, a series of experiments are planned at various scales and levels of venture involvement. These vary from those that involve a subset of labs and/or LYNM ventures (e.g., small experiments), to full quad-lab LYNM Program field-scale integrated experiments. Such experiments may involve chemical explosions with tracer materials or other means of simulating the expected signals from a nuclear explosion. The LYNM Program does not conduct actual nuclear explosions. Since 1992, the U.S. has observed a moratorium on underground nuclear explosions. This document is intended to provide the underlying scientific basis for the LYNM planned experimental work. Each specific LYNM experiment will develop a goals, objectives, and requirements (GOR) plan following the guidance in this document. The LYNM technical staff will define the numbers and types of experiments required over the course of the Program based on technical needs and within funding constraints. As with any scientific experiment series, the number and types of experiments may change based upon the experimental results obtained. An experiment that agrees with models/codes/software signature predictions may need fewer repetitions/variations, depending upon the level of statistical rigor desired, as compared to one in which the predictions and experimental data do not match. The large LYNM field-scale integrated experiments require the longest lead-time for planning, and these are discussed in more detail near the end of this document.

58 GEOSCIENCES↗

DOE OSTI2023

Compaction of crushed salt for safe containment – a summary of the KOMPASS projects

Abstract. For the underground disposal of high-level nuclear waste in rock salt formations, the safety concept includes the backfilling of open cavities with crushed salt. For the prognosis of the sealing function of the backfill for the safe containment of the radioactive waste, it is crucial to have a comprehensive process understanding of the crushed-salt compaction behavior. The crushed-salt compaction process is influenced by internal properties (e.g., grain size, mineralogy, and moisture content) and boundary conditions (e.g., temperature, stress state, and compaction rate) and, therefore, involves several coupled thermal–hydro–mechanical (THM) processes (Hansen et al., 2014; Kröhn et al., 2017). With the paradigm shift from the limited release of radionuclides to safe containment due to the German Repository Site Selection Act passed in 2017, the importance of crushed salt as geotechnical barrier has increased, with a focus on the evolution of its hydraulic properties. Based on the knowledge gaps in the current process understanding, the “Compaction of crushed salt for safe containment” (KOMPASS) projects were initiated to improve the scientific basis behind using crushed salt for the long-term isolation of high-level nuclear waste within rock salt repositories. The efforts to improve the prediction of crushed-salt compaction begun during the first phase of the KOMPASS projects (Czaikowski et al., 2020) and were followed up in a second phase ending in June 2023. The primary achievements of the projects are as follows (Czaikowski et al., 2020; Friedenberg et al., 2022): specification of the KOMPASS reference material, an easily available and reproducible synthetic crushed-salt material, for generic investigations; development of pre-compaction methods and successful production of samples in the short term and under in situ loading conditions; formulation of an extended laboratory program addressing the isolated investigation of known relevant factors influencing the compaction behavior of crushed salt (Düsterloh et al., 2022); execution of long-term compaction tests addressing isotropic and deviatoric load changes, temperature, and compaction state; construction of a backfill body using the KOMPASS reference material in the Sondershausen mine through collaboration with the SAVER (Entwicklung eines salzgrusbasierten Versatzkonzepts unter der Option Rückholbarkeit) project (Schaarschmidt and Friedenberg, 2022); advancement of the tools for microstructure investigation methods (Svensson and Laurich, 2022); generation (first stages) of a microphysical process list combining literature research with our own findings; benchmarking of long-term compaction test for model development and optimization of various existing models as well as the development of new models; application of a virtual demonstrator (2D model representing a backfilled drift in rock salt) for the visualization of developments and the quantification of the models (Rabbel, 2022). In summary, the KOMPASS projects contributed to the reduction of uncertainties and the strengthening of the safety case for using crushed salt within rock salt repositories.

Friedenberg, Larissa↗

DOE OSTI2025

Seismic monitoring of underground vibration: database of seismic data and ground truth

Seismic waves provide valuable insights into underground activities, serving as an essential tool for monitoring anomalies that could signal containment breaches in geological repositories. We aim to test and refine underground detection and geolocation techniques to identify anomalous vibration signals indicative of potential breaches, thereby strengthening georepository safeguards. We evaluate the effectiveness of two distinct, low-maintenance sensing technologies (surface geophones and underground distributed acoustic sensing (DAS) fiber optic cable) leveraging existing datasets. This report details the experimental designs, instrumentation, and data characteristics for both seismic and DAS arrays. Additionally, we provide a ground truth database documenting relevant operational activities for each experiment.

58 GEOSCIENCES↗

DOE OSTI2023

Scaling Containment on a Large Centrifuge

Containment science concerns the trapping or leakage of radioactive cavity gases from underground nuclear explosions (UNEs). The most physically relevant data for validation of containment science comes from legacy UNE testing or large field-scale chemical explosions. Field-scale tests can inform on the degree of residual stress imparted to host geology and possible formation of an accompanying gas-containing “stress cage”, for example, as a function of chemical explosion yield. However, field testing can be expensive, difficult to conduct, and challenging to instrument with limitations on data coverage (i.e., the number of boreholes; difficult coring through damage zones). Small-scale laboratory tests are typically simpler to conduct and more thoroughly characterize, but may not include the right scale of containment processes for stress-cage or chimney formation. This report presents the theory and fundamentals of large centrifuge physical modeling, including a history of explosive or similar testing relevant to containment science investigations on centrifuges. Subscale models with embedded chemical explosives in the enhanced gravity of a large centrifuge can represent hundreds of meters of depth and large explosions not otherwise attainable in the laboratory as based on scaling of length, energy, and other processes by the g-factor of the centrifuge (i.e., the number of times larger the centrifugal force is than the gravitational force on the Earth’s surface). The centrifuge uniquely joins the simplicity and exhaustiveness of laboratory-scale characterization with the physics of field-scale processes. This report is part of Sandia National Laboratories’ (SNL’s) effort to prepare for physical modeling with approximately one-meter tall geologic models of stress cage and/or chimney formation on its 29-foot [8.84 m] radius centrifuge with a load capacity of 1.6 million 𝑔-pounds [726 𝑔-ton]. The scaling relationships herein will inform model design decisions and performance requirements for in-flight sensors.

42 ENGINEERING↗

DOE OSTI2025

Evaluation of Hanford Supernatant Waste Evaporation

• Hanford site in Washington has 27 underground “double-shell” storage tanks containing radioactive waste. Storage space is utilized to max capacity. • Construction of new tanks is undesirable, but volume reduction is still possible by vacuum evaporation of liquid waste. • Excess evaporation may create additional problems in solids precipitation, waste density and corrosivity. • Evaporation of liquid waste was simulated to determine possible outcomes.

Barkai, Benjamin [Savannah River National Laborato↗

DOE OSTI2021

Testbeds for test Readiness: Strategic Snapshot

Test bed engineering, monitoring for underground explosive and nuclear testing will be needed if the United States returns to a test posture of nuclear device testing. To maintain and rebuild the capability of test readiness, agile cost-effective test beds are needed and LANL as well as NNSS are the perfect locations to do this. Shallow and deep boreholes should be created to research containment science, diagnostic placement and optimization, coupling and emplacement science, tracer use for fracture and cratering research, and validation of test article performance.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗