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At least 19 records

Explosive Byproduct Gas Transport Through Sorptive Geomedia

Current underground nuclear explosion (UNE) detection strategies rely heavily on atmospheric noble gas sampling of radioxenon. However, discriminating nuclear weapons testing programs from civilian sources is difficult due to highly variable atmospheric radioxenon backgrounds and processes affecting subsurface transport of parent radionuclides. Here, we aim to study the transport of gases produced by subsurface explosions as novel stable signatures for underground nuclear explosion (UNE) monitoring. These gases may be produced in large quantities with distinct molecular ratios, which will be impacted by subsurface transport processes. To demonstrate how ratios of gases produced by explosions can change during transport in geomaterials, we conducted laboratory benchtop experiments on the transport of carbon dioxide (CO 2 ) and hydrogen (H 2 ) gases through variably saturated zeolitic tuff, which is abundant at the historic US testing site. We observed that zeolitic tuff sorbs substantial quantities of CO 2 while allowing H 2 to transport more freely, leading to changes in the molecular ratios of the two gases along the transport pathway. Gas uptake in the dry zeolitic tuff core was 72.3% for CO 2 , compared with 53.4% for xenon and 7.6% for H 2 . The presence of 20% water saturation disrupted the CO 2 sorption process, though to a lesser extent than observed for noble gases, with a 36.7% drop in xenon sorption compared with a 21.9% drop for CO 2 . These results represent the first observations of zeolite sorption altering explosive gas ratios during transport through geomedia relevant to nuclear proliferation monitoring.

54 ENVIRONMENTAL SCIENCES↗

Permeability scaling relationships of volcanic tuff from core to field scale measurements

A recent chemical explosive test in P-Tunnel at the Nevada National Security Site, Nevada, USA, was conducted to better understand how signals propagate from explosions in the subsurface. A primary signal of interest is the migration of gases that can be used to differentiate chemical from nuclear explosions. Gas migration is highly dependent on the rock permeability which is notoriously difficult to determine experimentally in the field due to a potentially large dependence on the scale over which measurements are made. Here, we present pre-explosion permeability estimates to characterize the geologic units surrounding the recent test. Permeability measurements were made at three scales of increasing size: core samples (≈2 cm), borehole packer system tests (≈1 m), and a pre-shot cavity pressurization test (> 10 m) across ten tuff units. Permeability estimates based on core measurements showed little difference from borehole packer tests. However, permeability in most rock units calibrated from cavity pressurization tests resulted in higher permeability estimates by up to two orders of magnitude. Here, we demonstrate that the scale of the measurement significantly impacts the characterization efforts of hydraulic properties in volcanic tuff, and that local-scale measurements (< 10 m scale) do not incorporate enough heterogeneity to accurately predict field-scale flow and mass transport.

Environmental sciences↗

Method Validation Summary for L16.2 AD-ISO-0015 for ISO-17025 / NFAC Applications

Methods for the analysis of semi-volatile organic compounds are employed at Savannah River National Laboratory (SRNL) for routine and non-routine samples from tank waste, process control, waste acceptance, and a wide array of other process and research samples. A method has been developed by SRNL, based on existing methods for semi-volatile analysis, for the analysis of nitroaromatic high explosives by gas chromatography / mass spectrometry in soils and sediments. Relative to past work performed at SRNL on nitroaromatic explosives, this developed, optimized, and validated method can achieve lower limits of detection and quantitation, greater precision, lower bias, higher linearity, and accuracy across a greater linear range.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Predicting multiphase flow and tracer transport for an underground chemical explosive test

Detecting radionuclide gas seepage from clandestine underground nuclear tests is central to nonproliferation explosion monitoring research. Yet, early-time (<6 day) gas transport driven by the explosive pressure wave remains poorly constrained due to scarcity of field data. We simulate multi-phase gas transport in the vadose zone using pre-shot data from a recent chemical explosion in P-Tunnel at the Nevada National Security Site, USA. Despite using a simplified 2D-radial model, predictions of tracer arrival matched observations within one order-of-magnitude. Our results show how transient blast forcing rapidly mobilizes gases from the cavity into surrounding rock – critical for optimizing sensor placement and test planning. This unique integration of field data and modeling represents a significant improvement in our ability to predict gas migration from underground explosions. More broadly, it offers insights into the coupled dynamics of pressure waves and contaminant transport in the vadose zone, with implications for monitoring and hazard assessment.

54 ENVIRONMENTAL SCIENCES↗

An In Situ , Automated High-Explosives Aging Method Utilizing Two-Dimensional Gas Chromatography–Mass Spectrometry

Understanding chemical changes that occur in high explosives as they age is of great importance to the safe employment and storage of these compounds. Traditional methods of aging high explosives even under accelerated aging conditions are time intensive with durations on the order of months to years. The nature of traditional aging analyses reduces each sample to a snapshot data point often separated widely in time, requiring many assumptions as to how the degradation products develop. Further complicating matters, several analytical techniques are typically employed for each sample analysis in order to ascertain an entire picture of the decomposition pathways. To address these shortcomings with existing methods, a new method of accelerated aging of high explosives utilizing comprehensive two-dimensional gas chromatography coupled to high-resolution mass spectrometry (GC × GC-HRMS) was developed using 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (CL-20) as a model compound for method development. This in situ automated method reduces the time scale of aging to a matter of hours using the inlet of the GC × GC as the aging vessel. GC × GC in combination with HRMS allowed for the collection of both evolved gases and other decomposition products produced during the entire aging process in real time with HRMS providing far greater certainty in identification of explosives aging products. Additionally, this method allowed for a higher throughput of samples with greatly simplified sample preparation. Chemometric analysis of the GC × GC-HRMS data set via the alteration analysis (ALA) enabled discovery of statistically significant chemical changes providing insight into the variation of decomposition pathways with varying aging temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Removal and Deactivation of Bond Sodium from Fast Reactor Blanket Materials

The disposition of sodium-bonded spent nuclear fuel and blanket materials in a repository is complicated by the presence of sodium metal that is used as a thermal bond between the uranium metal fuel and blanket slugs and their cladding. The concern is that the metallic sodium could react with water, producing explosive hydrogen gas, or could exhibit a pyrophoric character. Thus, experimental studies were performed to investigate and demonstrate the removal and deactivation of bond sodium from blanket material in a dry environment. Specifically, bond sodium was removed from unirradiated Fermi-1 blanket elements and an assembly via a melt-drain-evaporate process using elevated temperature and reduced pressure. The effectiveness of sodium metal removal from the blanket materials and their associated cladding was =99.9998%, based on post-test quantitative analyses. The separated sodium metal was collected and subsequently deactivated by reacting it in a molten state with a controlled addition of ammonium chloride particles atop a molten salt medium. In this process sodium chloride is formed and assimilates into the salt pool. The subsequent deactivation of the bond sodium produced a solid ingot of sodium chloride, potassium chloride, lithium chloride, and cesium chloride that was devoid of sodium metal based on post-test analyses of the salt product. Both the sodium removal and deactivation operations were conducted within a dry inert atmosphere enclosure. The results of this study substantiate a path forward for the disposition of sodium-bonded blanket materials, including 34 metric tons heavy metal in irradiated Fermi-1 blanket material currently stored at Idaho National Laboratory.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Quantifying the Potential of Argon Detection Capabilities for Nuclear Explosion Monitoring

Abstract Current noble gas detection systems for nuclear explosion monitoring are based on the detection of four radioxenon isotopes—Xe-131m, -133, -133m and -135. The data provided by radioxenon detection could be enhanced by other radionuclide signatures such as Ar-37. Activation of Ca-40 in rock by neutrons produces Ar-37, and monitoring for this additional nuclide could help distinguish detections of nuclear explosions from background sources, such as medical isotope production. This work studies the capabilities of a hypothetical argon detection network. A 10 kt explosion was modeled using MCNP and SCALE to determine the inventory of Ar-37 created in a representative granite rock layer, assuming either 0.1, 1 or 10% of the total inventory was released. The Ar-37 inventory was combined with atmospheric transport data from HYSPLIT compiled in a previous study, along with the detection limits of standard Ar-37 detection systems, to determine how many hypothetical monitoring stations would detect Ar-37 from an explosion. This method was repeated for 365 HYSPLIT data sets to create a year’s worth of hypothetical explosions, releases, and detections. The study quantified the average number of detections per release, the number of stations detecting Ar-37, and the possibility of detecting Ar-37 in coincidence with xenon.

37Ar↗

Using Radiogenic Noble Gas Nuclides to Identify and Characterize Rock Fracturing

Abstract Fracture‐released radiogenic noble gas nuclides are used to identify locations and constrain the volume of new fracture creation during subsurface detonations. Real‐time, in situ noble gases and reactive gases were monitored using a field‐deployed mass spectrometer and automated sampling system in a multilevel borehole array. Released gases were measured after two different detonations having distinct energy, pressure, and gas volume characteristics. Explosive‐derived gases (N 2 O, CO 2 ) and excess radiogenic 4 He and 40 Ar above atmospheric background are used to identify locations of gas transport and new fracture creation after each detonation. Fracture‐released radiogenic 4 He is used to constrain the volume of newly created fractures with a model of helium release from fracturing. Explosive by‐product gas was observed in multiple locations both near and distal to the shot locations for both detonations. Radiogenic 4 He and 40 Ar release from rock damage was observed in locations near the detonation after the second, more powerful detonation. Observed 4 He response is consistent with a model of diffusive release from newly created fractures. Volume of new fractures estimated from the 4 He release ranges from 1 to 5 m 2 with apertures ranging from 0.1 to 1 m. Our results provide evidence that radiogenic noble gases released during fracture creation can be identified at the field scale in real time and used to identify timing and location of fracture creation during deformation events. This technique could be useful in subsurface science and engineering problems where the location and amount of newly created rock fracturing is of interest including fault rupture, mine safety, subsurface detonation monitoring and reservoir stimulation.

58 GEOSCIENCES↗

Assessing the Potential Impact of Fugitive Methane Emissions on Offshore Platform Safety

One of the biggest risks to safety on offshore platform safety is the ignition of high-pressure natural gas streams. Currently, the size and number of fugitive emissions on offshore platforms is unknown and methods used to detect fugitives have significant shortcomings. To investigate the frequency, size, and potential impact of fugitives, a data collection exercise was conducted using incidents reported, leak survey data, and independent measurements. The size and number of fugitives on offshore facilities were simulated to investigate likely areas of safety concern. Incident reports indicate in 2021 there were 113 reports of gas leaks on 1119 offshore facilities, suggesting 0.02 fugitives per Type 1 facility (older, shallow-water platforms) and 0.31 fugitives per Type 2 facility (larger deeper-water facilities). Leak survey data report 12 fugitives per Type 1 facility (average emission 0.6 kg CH 4 h −1 leak −1 ) and 15 fugitives per Type 2 facility (average emission 1.5 kg CH 4 h −1 leak −1 ). Reconciliation of direct measurements with a bottom-up model suggests that the number of fugitive emissions generated from the leak report data is an underestimate for Type 1 platforms (44 fugitives facility −1 ; average emission 0.6 kg CH 4 h −1 leak −1 ) and in general agreement for the Type 2 platforms (15 fugitives facility −1 ; average emission 1.5 kg CH 4 h −1 leak −1 ). Analysis of the fugitive emission rates on an offshore platform suggests that gas will not collect to explosive concentration if any air movement is present (>0.36 mph); however, large volumes of air (~600 m 3 ) near representative leaks on the working deck could become explosive in hour-long zero-wind conditions. We suggest that wearable technology could be employed to indicate gas build up, safety regulations amended to consider low-wind conditions and real-world experiments are conducted to test assumptions of air mixing on the working deck.

explosion↗

Partially Ionized Plasma Physics and Technological Applications

Partially ionized plasma physics has attracted increased attention recently due to numerous technological applications made possible by the increased sophistication of computer modelling, the depth of the theoretical analysis, and the technological applications to a vast field of manufacturing for computer components. Partially ionized plasma is characterized by a significant presence of neutral particles in contrast to the fully ionized plasma. The theoretical analysis is based upon solutions of the kinetic Boltzmann equation, yielding the non-Maxwellian electron energy distribution function (EEDF), thereby emphasizing the difference with a fully ionized plasma. The impact of the effect on discharges in inert and molecular gases is described in detail, yielding the complex nonlinear phenomena resulting in plasma selforganization. A few examples of such phenomena are given, including the non-monotonic EEDFs in the discharge afterglow in a mixture of argon with the molecular gas NF3; the explosive generation of cold electron populations in capacitive discharges, hysteresis of EEDF in inductively coupled plasmas. Recently, highly advanced computer codes were developed in order to address the outstanding challenges in plasma technology. These developments are briefly described in general terms.

non-Maxwellian electron energy distribution functi↗

A multi-Physics Experiment for Low-Yield Nuclear Explosion Monitoring

A series of multi-physics experiments, referred to as Physics Experiment 1 (PE1) is underway at the United States’ Nevada National Security Site (NNSS). The PE1 series includes detonations of three underground chemical explosions in P-tunnel, with fully coupled (PE1 A), partially decoupled (PE1 D L ), and fully decoupled (PE1 B) emplacements. Canisters with gas tracers are imbedded in the explosives, and the tracers are released when the canister is destroyed by the detonation. A dedicated electromagnetic (EM) experiment (EMX) generates well-characterized EM signals at an underground location near the chemical explosive experiments. A series of atmospheric experiments (METEX, REACT, and METREX) release smoke and radioactive tracers around Aqueduct Mesa to test gas transport in complex topography. Each of the chemical explosive experiments includes a network of sensors to record seismic, acoustic, and electromagnetic waves, measurement of atmospheric conditions, and air sample collection for measurement of tracer concentration. EMX records EM signals underground and on the surface of Aqueduct Mesa. METEX, REACT, and METREX include measurement of atmospheric condition, as well as tracking smoke releases. REACT and METREX add low-level radioactive gas tracers to the atmospheric releases.

58 GEOSCIENCES↗

Description of the Gas Sampling and Circulation System for the LYNM PE1-A Experiment

A series of multiphysics experiments, referred to as Physics Experiment 1 (PE1) is underway at the U.S. Nevada National Security Site. The PE1 series includes detonations of three underground chemical explosions. As the name implies, there are a number of experiments investigating the signals generated by the explosion. The experiment series objectives are outlined in a report from Lawrence Livermore National Laboratory.1 One of the experiments is a gas migration experiment. Gas tracers were imbedded in the explosives and gas sampling boreholes were installed in the formation in the test bed. Connected to the monitoring points is a circulation system that moves gas to a central measurement location. This report does not describe the gas analysis or collection systems, but rather the circulation system that provides the gas for measurement. Here, we have combined four project documents into a single report that describes the design, build, installation, testing, and operation of the gas sampling network.

42 ENGINEERING↗

A comparison of long-term 37 Ar and 39 Ar transport and implications for 39 Ar as a persistent indicator of underground nuclear explosions

Measurements were first made in 2016 of legacy 39 Ar gas from the decades-old Barnwell underground nuclear explosion site within the Nevada National Security Site. This has raised the question of the ubiquity of the radionuclide 39 Ar following underground nuclear explosions in general locations. This article presents a high-level evaluation of the scientific case for using 39 Ar as a long-term indicator of underground nuclear explosions. Assessment is made based on a broad set of assumptions to reasonably estimate the persistence of 39 Ar in the subsurface environment following an explosion to establish potential detectability years to decades after the originating event.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Effect of a collapsing gas bubble on the shock-to-detonation transition in liquid nitromethane

We studied the shock-induced collapse of butane gas bubbles in the homogeneous explosive nitromethane (NM) to investigate the effects of hot spot formation on the detonation process. A butane bubble was injected into a sample of NM, and a shock wave from a flat plate impactor compressed the bubble, creating a localized hot spot. We measured shock and detonation wave speeds with optical velocimetry, and we used a high-speed camera to image the shock propagation and bubble collapse processes. A multiband optical fiber pyrometer measured the time-resolved thermal radiance, and we used the results and emissivity values extracted from spectral fits to estimate temperatures. We measured the characteristics of the shock-to-detonation transition in NM with and without a bubble. All experiments were performed at shock pressures near 8 GPa, where neat NM can detonate. A single bubble in this system was shown to sensitize NM, leading to a reduced run-to-detonation time. We used hydrodynamic modeling to predict shock wave propagation, the extent of chemical reaction, and subsequent temperature rise from the collapsing bubble. We used a temperature-dependent Arrhenius burn model for simulations, and it yielded much better results than reactive burn models that depend only on pressure and density.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Preferential adsorption of noble gases in zeolitic tuff with variable saturation: A modeling study of counter-intuitive diffusive-adsorptive behavior

Noble gas transport through geologic media has important applications in the prediction and characterization of measured gas signatures related to underground nuclear explosions (UNEs). Retarding processes such as adsorption can cause significant species fractionation of radionuclide gases, which has implications for measured and predicted signatures used to distinguish radioxenon originating from civilian nuclear facilities or from UNEs. Accounting for the effects of variable water saturation in geologic media on tracer transport is one of the most challenging aspects of modeling gas transport because there is no unifying relationship for the associated tortuosity changes between different rock types, and reactive transport processes such as adsorption that are affected by the presence of water likewise behave differently between gas species. In this study, we perform numerical diffusive-adsorptive transport simulations to estimate gas transport parameters associated with bench-scale laboratory diffusion cell experiments measuring breakthrough in zeolitic and non-zeolitic rocks for a gaseous mixture of xenon, krypton, and SF 6 at varying degrees of water saturation (S w ). Counter-intuitive transport behavior was observed in the zeolitic rock experiments whereby breakthrough concentrations were significantly higher when the core was partially saturated (S w = 17 %) than under dry (S w = 0 %) conditions. Breakthrough of xenon was especially retarded in the dry core – likely due to comparatively high affinity of xenon for zeolitic adsorption sites – and estimated effective diffusion coefficients for all gases were approximately an order of magnitude lower than what is predicted by porosity-tortuosity models. We propose the counter-intuitive behavior observed is because water infiltration of zeolite nanopores reduces both the adsorptive capacity of the rock and the tortuosity of connected flow paths. We developed a two-site competitive kinetic Langmuir adsorption reaction for the porous media transport simulator in order to constrain transport parameters within zeolitic tuff, where differential adsorption to zeolite and non-zeolite pores was observed. We determined that liquid saturation-dependent diffusive-adsorptive transport is affected by subtle and at times competing processes that are specific to different gases, which have a significant overall influence on effective transport parameters.

58 GEOSCIENCES↗

Quantifying fission gas adsorption onto natural clinoptilolite in the presence of environmental air and water

Adsorption of noble gas fission products onto naturally occurring minerals is of interest for its potential to retain or retard emissions from nuclear fuel reprocessing operations or underground nuclear explosions. However, experimental studies of trace noble gas adsorption in the presence of air and water have largely focused on synthetic materials, such as activated carbon or metal-organic frameworks. Here, in this study, adsorption of Kr and Xe onto the naturally occurring zeolitic mineral clinoptilolite is studied in the presence of nitrogen and water. By varying the composition of the gas phase and monitoring the change in the combined adsorbate mass, the adsorbed concentration of noble gas is calculated gravimetrically. For dry clinoptilolite, the concentration of adsorbed Kr and Xe is linearly correlated with noble gas pressure and Henry's Law appears satisfactory, despite the presence of nitrogen at atmospheric pressures. However, the presence of water significantly reduces the adsorbed concentration of both Kr and Xe, which is typical in nanoporous sorbents. Here, an empirical bivariate model is presented, combining the Henry's Law adsorption model for a dry adsorbent with the exponential reduction in the presence of water, as reported by Lungu and Underhill in 1999. This model provides a means to estimate the adsorbate concentration at the trace partial pressures and higher water contents relevant to field-scale modeling of fission gas transport through the vadose zone.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A flow-through gamma detection system for sub-surface radioxenon tracer measurements in LYNM PE1

A continuous flow-through, real-time radioxenon sensor array has been designed to monitor either 127 Xe or 133 Xe tracer gas as part of a series of underground chemical explosions in the Low-Yield Nuclear Monitoring (LYNM) Physics Experiment 1 (PE1). The sensors are pairs of shielded thallium-doped sodium iodide gamma-ray detectors that surround a gas measurement chamber. Each measurement chamber is connected to a sampling location in the geology surrounding the chemical explosion or in the access tunnel. The first experiment in the series, PE1 A, occurred in 2023 and the system quantified the 127 Xe tracer gas in the gas sampling lines for four weeks following the experiment execution. The array generated a set of radioxenon concentration time series with a 15-minute resolution that will be used to refine subsurface gas transport models.

Gamma-ray coincidence detection↗