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Effects of hydrogen isotope type on oxidation rates for trace releases

Fire Safety Journal

Shurtz, Randy S.; Brown, Alexander B.; Takahashi, Lynelle K.; Coker, Eric N.

The fraction of tritium converted to the water form in a fire scenario is one of the metrics of greatest interest for radiological safety assessments. The conversion fraction is one of the prime variables contributing to the hazard assessment. This paper presents measurements of oxidation rates for the non-radioactive hydrogen isotopes (protium and deuterium) at sub-flammable concentrations that are typical of many of the most likely tritium release scenarios. These measurements are fit to a simplified 1-step kinetic rate expression, and the isotopic trends for protium and deuterium are extrapolated to produce a model appropriate for tritium. The effects of the new kinetic models are evaluated via CFD simulations of an ISO-9705 standard room fire that includes a trace release of hydrogen isotope (tritium), illustrating the high importance of the correct (measurement-based) kinetics to the outcome of the simulated conversion.

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Flammability and dispersion of tritium in confined release scenarios

Shurtz, Randy S.; Brown, Alexander B.; Takahashi, Lynelle K.

Ignition of a flammable tritium-air mixture is the most probable means to produce the water form (T2O or HTO), which is more easily absorbed by living tissue and is hence ~10,000 times more hazardous to human health when uptake occurs compared to the gaseous form (T2 or HT; per Mishima and Steele, 2002). Tritium-air mixtures with T2 concentrations below 4 mol% are considered sub-flammable and will not readily convert to the more hazardous water form. It is therefore desirable from a safety perspective to understand the dispersion behavior of tritium under different release conditions, especially since tritium is often stored in quantities and pressures much lower than is typical for normal hydrogen. The formation of a flammable layer at the ceiling is a scenario of particular concern because the rate of dispersion to nonflammable conditions is slowest in this configuration, which maximizes the time window over which the flammable tritium may encounter an ignition source. This report describes the processes of buoyant rise and dispersion of tritium. Accumulation of flammable concentrations of tritium next to the ceiling is a common safety concern for hydrogen, but this situation can only occur if dispersion rates are slow with respect to rates of release and rise. Theory and simulations demonstrate that buoyancy does not cause regions with flammable concentrations to form within buildings from sources that have previously been mixed to sub-flammable concentrations. A simulated series of tritium release events with their associated dispersion behavior are reported herein; these simulations apply computational fluid dynamics to rooms with three different ceiling heights and a variety of tritium release rates. Safety related quantities from these simulations are reported, including the mass and volume of tritium occurring in a flammable mixture, the presence or absence of a flammable layer at the ceiling, and the time required for dispersion to nonflammable conditions after the end of the tritium release event. These safety metrics are influenced by the magnitude and rate of the tritium release with respect to the air volume in the room and also the momentum of the plume or jet with respect to the ceiling height. Several screening criteria are recommended to assess whether a specific tritium release scenario is likely to form a flammable layer at the ceiling. The methods and results in this modeling study have applicability to explosion safety analysis for other buoyant flammable gases, including the lighter isotopes of hydrogen.

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HAZARD ASSESSMENT OF FIRE CONSEQUENCES FROM A FUEL STORAGE EXPLOSION

Proceedings of the Thermal and Fluids Engineering Summer Conference

Brown, Alexander B.; Shurtz, Randy S.; Wilke, Jason W.

Two relatively under-reported facets of fuel storage fire safety are examined in this work for a 250, 000 gallon two-tank storage system. Ignition probability is linked to the radiative flux from a presumed fire. First, based on observed features of existing designs, fires are expected to be largely contained within a designed footprint that will hold the full spilled contents of the fuel. The influence of the walls and the shape of the tanks on the magnitude of the fire is not a well-described aspect of conventional fire safety assessment utilities. Various resources are herein used to explore the potential hazard for a contained fire of this nature. Second, an explosive attack on the fuel storage has not been widely considered in prior work. This work explores some options for assessing this hazard. The various methods for assessing the constrained conventional fires are found to be within a reasonable degree of agreement. This agreement contrasts with the hazard from an explosive dispersal. Best available assessment techniques are used, which highlight some inadequacies in the existing toolsets for making predictions of this nature. This analysis, using the best available tools, suggests the offset distance for the ignition hazard from a fireball will be on the same order as the offset distance for the blast damage. This suggests the buy-down of risk by considering the fireball is minimal when considering the blast hazards. Assessment tools for the fireball predictions are not particularly mature, and ways to improve them for a higher-fidelity estimate are noted.

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SIMULATING THE PLUME QUENCH FOR PLASMA SPRAY APPLICATIONS

Proceedings of the Thermal and Fluids Engineering Summer Conference

Brown, Alexander B.; Vackel, Andrew V.

Plasma sprays can be used to melt particles, which may be deposited on an engineered surface to apply unique properties to the part. Because of the extreme temperatures (>>3000ºC) it is desirable to conduct the process in a way to avoid melting the parts to which the coatings are being applied. A jet of ambient gas is sometimes used to deflect the hot gases, while allowing the melted particles to impact and adhere to the substrate. This is known as a plume quench. While plume quenching is done in practice, to our knowledge there have not been any studies on how to apply a plume quench, and how it may affect the flows. We have recently adapted our fire simulation tool to simulate argon plasma sprays with a variety of metal particles. Two nozzle conditions are considered, with very different gas flow and power conditions. Two particle types are considered, Tantalum and Nickel. For the model, the k-epsilon turbulence model is compared to a more dynamic TFNS turbulence model. Limited data comparisons suggest the higher-fidelity TFNS model is significantly more accurate than the k-epsilon model. Additionally, the plume quench is found to have a noticeable effect for the low inlet flow case, but minimal effect on the high flow case. This suggests the effectiveness of a quench relates to the relative momentum of the intersecting gas jets.

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Smoke Measurements from a High-flux Ignition Experiment

Proceedings of the Thermal and Fluids Engineering Summer Conference

Brown, Alexander B.; Cruz-Cabrera, A.A.; Travis Bateman, Jessica A.

Smoke may be defined as the particulate products from fire and is composed of organics originating from unburnt fuel and soot, which is mostly carbon and is formed in the rich side of the flame. The fire community regularly measures smoke emissions using the cone calorimeter (CC) and the fire propagation analyzer (FPA) devices via laser extinction. Their measurements are conducted over the burn time of the material, generally minutes. Our high-flux exposures from concentrated solar irradiance result in emissions lasting only a few seconds. We have adapted the historical methods to our application to permit similar quantitative assessments of smoke. We illustrate here our modified procedure and present some results of the testing performed by exposing materials to concentrated solar energy. An assessment of the uncertainty in the smoke yield measurements is made. The data are expected to contribute to the body of knowledge on the emissions of smoke from ignitions caused by more unconventional initiating events involving very high heat fluxes.

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HAZARD ASSESSMENT OF FIRE CONSEQUENCES FROM A FUEL STORAGE EXPLOSION

Proceedings of the Thermal and Fluids Engineering Summer Conference

Brown, Alexander B.; Shurtz, Randy S.; Wilke, Jason W.

Two relatively under-reported facets of fuel storage fire safety are examined in this work for a 250, 000 gallon two-tank storage system. Ignition probability is linked to the radiative flux from a presumed fire. First, based on observed features of existing designs, fires are expected to be largely contained within a designed footprint that will hold the full spilled contents of the fuel. The influence of the walls and the shape of the tanks on the magnitude of the fire is not a well-described aspect of conventional fire safety assessment utilities. Various resources are herein used to explore the potential hazard for a contained fire of this nature. Second, an explosive attack on the fuel storage has not been widely considered in prior work. This work explores some options for assessing this hazard. The various methods for assessing the constrained conventional fires are found to be within a reasonable degree of agreement. This agreement contrasts with the hazard from an explosive dispersal. Best available assessment techniques are used, which highlight some inadequacies in the existing toolsets for making predictions of this nature. This analysis, using the best available tools, suggests the offset distance for the ignition hazard from a fireball will be on the same order as the offset distance for the blast damage. This suggests the buy-down of risk by considering the fireball is minimal when considering the blast hazards. Assessment tools for the fireball predictions are not particularly mature, and ways to improve them for a higher-fidelity estimate are noted.

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Release of Contaminants from Burning Liquids and Solids

Brown, Alexander B.; Pierce, Flint P.; Zepper, Ethan T.

This report details model development, theory, and a literature review focusing on the emission of contaminants on solid substrates in fires. This is the final report from a 2-year Nuclear Safety Research and Development (NSRD) project. The work represents progress towards a goal of having modeling and simulation capabilities that are sufficiently mature and accurate that they can be utilized in place of physical tests for determining safe handling practices. At present, the guidelines for safety are largely empirically based, derived from a survey of existing datasets. This particular report details the development, verification and calibration of a number of code improvements that have been implemented in the SIERRA suite of codes, and the application of those codes to three different experimental scenarios that have been subject of prior tests. The first scenario involves a contaminated PMMA slab, which is exposed to heat. The modeling involved a novel method for simulating the viscous diffusion of the particles in the slab. The second scenario involved a small pool fire of contaminated combustible liquid mimicking historical tests and finds that the release of contaminants has a high functionality with the height of the liquid in the container. The third scenario involves the burning of a contaminated tray of shredded cellulose. A novel release mechanism was formulated based on predicted progress of the decomposition of the cellulose, and while the model was found to result in release that can be tuned to match the experiments, some modifications to the model are desirable to achieve quantitative accuracy.

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Tritium Fires: Simulation and Safety Assessment

Brown, Alexander B.; Shurtz, Randy S.; Takahashi, Lynelle K.; Coker, Eric N.; Hewson, John C.; Hobbs, Michael L.

This is the Sandia report from a joint NSRD project between Sandia National Labs and Savannah River National Labs. The project involved development of simulation tools and data intended to be useful for tritium operations safety assessment. Tritium is a synthetic isotope of hydrogen that has a limited lifetime, and it is found at many tritium facilities in the form of elemental gas (T2). The most serious risk of reasonable probability in an accident scenario is when the tritium is released and reacts with oxygen to form a water molecule, which is subsequently absorbed into the human body. This tritium oxide is more readily absorbed by the body and therefore represents a limiting factor for safety analysis. The abnormal condition of a fire may result in conversion of the safer T2 inventory to the more hazardous oxidized form. It is this risk that tends to govern the safety protocols. Tritium fire datasets do not exist, so prescriptive safety guidance is largely conservative and reliant on means other than testing to formulate guidelines. This can have a consequence in terms of expensive and/or unnecessary mitigation design, handling protocols, and operational activities. This issue can be addressed through added studies on the behavior of tritium under representative conditions. Due to the hazards associated with the tests, this is being approached mainly from a modeling and simulation standpoint and surrogate testing. This study largely establishes the capability to generate simulation predictions with sufficiently credible characteristics to be accepted for safety guidelines as a surrogate for actual data through a variety of testing and modeling activities.

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AN EXPERIMENTAL AND MODELING STUDY OF OXIDATION OF HYDROGEN ISOTOPES AT TRACE CONCENTRATIONS

Proceedings of the Thermal and Fluids Engineering Summer Conference

Shurtz, Randy S.; Coker, Eric N.; Brown, Alexander B.; Takahashi, Lynelle K.

In accident scenarios involving release of tritium during handling and storage, the level of risk to human health is dominated by the extent to which radioactive tritium is oxidized to the water form (T2O or THO). At some facilities, tritium inventories consist of very small quantities stored at sub-atmospheric pressure, which means that tritium release accident scenarios will likely produce concentrations in air that are well below the lower flammability limit. It is known that isotope effects on reaction rates should result in slower oxidation rates for heavier isotopes of hydrogen, but this effect has not previously been quantified for oxidation at concentrations well below the lower flammability limit for hydrogen. This work describes hydrogen isotope oxidation measurements in an atmospheric tube furnace reactor. These measurements consist of five concentration levels between 0.01% and 1% protium or deuterium and two residence times. Oxidation is observed to occur between about 550°C and 800°C, with higher levels of conversion achieved at lower temperatures for protium with respect to deuterium at the same volumetric inlet concentration and residence time. Computational fluid dynamics simulations of the experiments were used to customize reaction orders and Arrhenius parameters in a 1-step oxidation mechanism. The trends in the rates for protium and deuterium are extrapolated based on guidance from literature to produce kinetic rate parameters appropriate for tritium oxidation at low concentrations.

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Validating a Fire Simulation Tool with a Large-scale Helium Plume Dataset

Proceedings of the Thermal and Fluids Engineering Summer Conference

Brown, Alexander B.; Hewson, John C.

Fires of practical interest are often large in scale and involve turbulent behavior. Fire simulation tools are often utilized in an under-resolved prediction to assess fire behavior. Data are scarce for large fires because they are difficult to instrument. A helium plume scenario has been used as a surrogate for much of the fire phenomenology (O'Hern et al., 2005), including buoyancy, mixing, and advection. A clean dataset of this nature makes an excellent platform for assessing model accuracy. We have been participating in a community effort to validate fire simulation tools, and the SIERRA/Fuego code is compared here with the historical dataset. Our predictions span a wide range of length-scales, and comparisons are made to species mass fraction and two velocity components for a number of heights in the core of the plume. We detail our approach to the comparisons, which involves some accommodation for the uncertainty in the inflow boundary condition from the test. We show evolving improvement in simulation accuracy with increasing mesh resolution and benchmark the accuracy through comparisons with the data.

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DNS/LES Study of Representative Wall-Bounded Turbulent Flows using SIERRA/Fuego

Koo, Heeseok; Hewson, John C.; Brown, Alexander B.; Knaus, Robert C.; Kurzawski, Andrew K.; Clemenson, Michael D.

This report summarizes a series of SIERRA/Fuego validation efforts of turbulent flow models on canonical wall-bounded configurations. In particular, direct numerical simulations (DNS) and large eddy simulations (LES) turbulence models are tested on a periodic channel, a periodic pipe, and an open jet for which results are compared to the velocity profiles obtained theoretically or experimentally. Velocity inlet conditions for channel and pipe flows are developed for application to practical simulations. To show this capability, LES is performed over complex terrain in the form of two natural hills and the results are compared with other flow solvers. The practical purpose of the report is to document the creation of inflow boundary conditions of fully developed turbulent flows for other LES calculations where the role of inflow turbulence is critical.

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Results 1–25 of 155
Results 1–25 of 155