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This book chapter describes the special processes involved in sampling the airborne effluents from nuclear faciities. The title of the book is Radioactive Air Sampling Methods. The abstract for this chapter was cleared as PNNL-SA-45941.
Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.
Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 ( 137 Cs) and xenon-133 ( 133 Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137 Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137 Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133 Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137 Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133 Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137 Cs and 133 Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τ e , calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τ e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer ( 133 Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol ( 137 Cs) tracer. As a result, this indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.
The charging of various airborne particles was investigated using single-particle levitation and charge-balance equations. Though radioactive decay and triboelectrification can induce charging, it is typically assumed that the aerosols in a radioactive plume will not carry significant charge at steady state since atmospheric particles can have their charge neutralized through the capture of adjacent counter-ions (i.e., diffusion charging). Here to assess this assumption, we directly measured the surface charge and charge density of various triboelectrically charged aerosols including radioactive uranium oxide (<1 μm), urban dust, Arizona desert dust, hydrophilic and hydrophobic silica nanoparticles, and graphene oxide powders using an electric field-assisted particle levitator in air. Of these particles, uranium oxide aerosols exhibited the highest surface charge density. Charge balance equations were employed to predict the average charge gained from radioactive decay as a function of time and to evaluate the effects of diffusion charging on triboelectrically charged radioactive and non-radioactive particles in the atmosphere. Simulation results show that particles, initially charged through triboelectrification, can be quickly discharged by diffusion charging in the absence of radioactive decay. Nevertheless, simulation results also indicate that particles can be strongly charged when they carry radionuclides. These experimental and simulation results suggest that radioactive decay can induce strong particle charging that may potentially affect atmospheric transport of airborne radionuclides.
The Scrubber System focuses on using HEPA filters and carbon filtration to purify the exhaust of a Nuclear Thermal Propulsion engine of its aerosols and radioactive particles; however, new technology may lend itself to alternate filtration options, which may lead to reduction in cost while at the same time have the same filtering, if not greater, filtering capabilities, as its predecessors. Extensive research on various types of filtration methods was conducted with only four showing real promise: ionization, cyclonic separation, classic filtration, and host molecules. With the four methods defined, more research was needed to find the devices suitable for each method. Each filtration option was matched with a device: cyclonic separators for the method of the same name, electrostatic separators for ionization, HEGA filters, and carcerands for the host molecule method. Through many hours of research, the best alternative for aerosol filtration was determined to be the electrostatic precipitator because of its high durability against flow rate and its ability to cleanse up to 99.99% of contaminants as small as 0.001 micron. Carcerands, which are the only alternative to filtering radioactive particles, were found to be non-existent commercially because of their status as a "work in progress" at research institutions. Nevertheless, the conclusions after the research were that HEPA filters is recommended as the best option for filtering aerosols and carbon filtration is best for filtering radioactive particles.
The current paper presents a simulation-based analysis of aerosol dispersion in the near-field and far-field of a generic, conceptual microreactor operating at pressures close to the ambient pressure; therefore, in the event of an accident that causes radionuclide leakage from the microreactor containment, the radionuclide particles are less likely to travel too far from the reactor, as opposed to conventional reactors. Accordingly, the presented work provides estimates of average and 95-percentile values of the relative effluent concentration. A parametric study is then performed to narrow down the parameters which affect the aerosol dispersion characteristics most significantly. Simulations were performed in the computer code ARCON96, and the parameters found to affect aerosol dispersion characteristics are the atmospheric stability class, and the distance between the release point and the receptor. It is recommended that the computer code RADTRAD be used to calculate actual dosage over distance, using the outputs from ARCON96 as inputs, along with reactor-specific core term inventories. (authors)
Accurate prediction of the atmospheric transport of debris particles relies heavily on our knowledge of the size distribution of the particles within a debris cloud. Assuming a fixed particle size during simulations is not always viable since the size distribution of the debris can change during transport. Various microphysical processes, such as aggregation and breakup, influence debris particles and dictate any changes to the size distribution. To track those changes that can occur, a population balance model can be adopted and instituted within a model framework. Nonetheless, many of the models that simulate the transport of radioactive debris following a device-driven fission incident have historically neglected to consider these processes. As such, this work describes our effort to develop a modeling framework capable of simulating the transport and deposition of a radioactive plume generated from a fission incident with a dynamic population balance including particle aggregation and breakup. Herein the impact of aggregation and breakup, individually and collectively, on the particle size distribution is explored using the developed framework. When simulating aggregation, for example, six mechanisms, including Brownian coagulation, the convective enhancement to Brownian coagulation, van der Waals-viscous force correction for Brownian coagulation, gravitational collection, turbulent inertial motion, and turbulent shear, are considered. Brownian coagulation and its corrections have, as one would expect, a large impact on relatively small aggregates. Aggregates with a diameter that is less than or equal to 1.0 μm, for instance, comprise 50.6 vol % of all aggregates in the absence of aggregation and 31.2 vol % when Brownian coagulation and its corrections are considered. Gravitational collection and, to a much lesser extent, turbulent shear and turbulent inertial motion are, conversely, of great importance to relatively large aggregates (i.e., diameter greater than 3.0 μm). Additionally, the individual effects of atmospheric and particle parameters, such as wind speed and particle density, are examined. Of the parameters examined, turbulent energy dissipation and aggregate fractal dimension (i.e., aggregate shape with lower values representing more irregular particles) were of substantial importance since both terms directly impact aggregate stability and, by extension, the breakup rate. Large-scale transport and deposition simulations in a dry atmosphere are also presented and discussed as a proof of concept.
This report is part of the planning process for the demolition of the 234-5Z, 236-Z, 242-Z, and 291-Z-1 structures at the Plutonium Finishing Plant (PFP) on the Hanford Site. Pacific Northwest National Laboratory (PNNL) supports the U.S. Department of Energy (DOE) and the CH2M HILL Plateau Remediation Company (CHPRC) demolition planning effort by making engineering estimates of potential releases for various potential demolition alternatives. This report documents an analysis considering open-air demolition using standard techniques. It does not document any decisions about the decommissioning approaches; it is expected that this report will be revisited as the final details of the demolition are developed.
In 2002, the EPA amended 40 CFR 61 Subpart H and 40 CFR 61 Appendix B Method 114 to include requirements from ANSI/HPS N13.1-1999 Sampling and Monitoring Releases of Airborne Radioactive Substances from the Stack and Ducts of Nuclear Facilities for major emission points. Additionally, the WDOH amended the Washington Administrative Code (WAC) 246-247 Radiation protection-air emissions to include ANSI/HPS N13.1-1999 requirements for major and minor emission points when new permitting actions are approved. A result of the amended regulations is the requirement to prepare a written technical basis for the radiological air emission sampling and monitoring program. A key component of the technical basis is the Potential Impact Category (PIC) assigned to an emission point. This paper discusses the PIC assignments for the Pacific Northwest National Laboratory (PNNL) Integrated Laboratory emission units; this revision includes five PIC categories.
This report presents estimates of dispersion coefficients and effective dose for potential air dispersion scenarios of uncontrolled releases from Oak Ridge National Laboratory (ORNL) buildings 3026C, 3026D, and 3140 prior to or during the demolition of the 3026 Complex. The Environmental Protection Agency (EPA) AERMOD system1-6 was used to compute these estimates. AERMOD stands for AERMIC Model, where AERMIC is the American Meteorological Society-EPA Regulatory Model Improvement Committee. Five source locations (three in building 3026D and one each in building 3026C and the filter house 3140) and associated source characteristics were determined with the customer. In addition, the area of study was determined and building footprints and intake locations of air-handling systems were obtained. In addition to the air intakes, receptor sites consisting of ground level locations on four polar grids (50 m, 100 m, 200 m, and 500 m) and two intersecting lines of points (50 m separation), corresponding to sidewalks along Central Avenue and Fifth Street. Three years of meteorological data (2006 2008) were used each consisting of three datasets: 1) National Weather Service data; 2) upper air data for the Knoxville-Oak Ridge area; and 3) local weather data from Tower C (10 m, 30 m and 100 m) on the ORNL reservation. Annual average air concentration, highest 1 h average and highest 3 h average air concentrations were computed using AERMOD for the five source locations for the three years of meteorological data. The highest 1 h average air concentrations were converted to dispersion coefficients to characterize the atmospheric dispersion as the customer was interested in the most significant response and the highest 1 h average data reflects the best time-averaged values available from the AERMOD code. Results are presented in tabular and graphical form. The results for dose were obtained using radionuclide activities for each of the buildings provided by the customer.7 Radiation dose was calculated assuming complete release of the building inventory as information was lacking regarding the portion of the building inventory expected to be released. Thus the results are derived using an extremely conservative release as documented in the Preliminary Hazard Screening report.7 To more closely approximate the result of a release, one must estimate the fraction of the total inventory released and multiply the results described above by that fraction. An example of how this calculation is accomplished is provided. Should an actual uncontrolled release occur, the results of this modeling effort could only be used to establish a rough order-of-magnitude for the event.
Release fractions are commonly used to make conservative estimates of emissions from processes and are applied to characterize industrial operations to safeguard workers and public. Release fractions cannot be derived theoretically; they must be measured. Appropriate measurements are limited. This paper describes tests that were conducted to provide large-scale release fraction data for estimating releases from three operations proposed for waste remediation at the Hanford Site in Richland, Washington. Experiments were conducted to measure release fractions of three processes: 1) pipe discharge of liquid and slurry in free fall into a liquid or slurry, 2) jet transfer of contents to the other side of the tank either impacting the tank wall or falling into the fluid pool, and 3) high pressure fan jet striking a steel plate or simulated waste from a small stand-off distance. The tests were conducted without forced ventilation in an enclosed prototypic ¼-scale model of a 3785 m^3 (1 million gallon) tank in use at the Hanford Site for storage of radioactive waste. Aerosol releases were characterized based on filter samples of aerosol collected near the process stream, tank wall, and tank top to determine release fraction at engineering scale. Particle size distribution measurements were analyzed to determine whether the particles were in the respirable range. The release fractions for the top of the unventilated tank ranged from 9x10-7 to 6x10-4 depending on the process simulated. The particle size distribution was determined to be log-normally distributed with geometric mean diameters ranging from 3 to 8 µm. Thus, all particles are conservatively considered to be “respirable.”
Deep bed sand (DBS) filters have filtered radioactive particulates at two United States Department of Energy (DOE) sites since 1948. Some early DBS filters experienced issues with chemical attack on support tiles, requiring significant repairs. Designs of DBS filters constructed since 1970 paid greater attention to chemical compatibility, resulting in decades of reliable performance since 1975.
Aerosol monitoring for radioactivity is a mature and proven technology. However, by improving key specifications of aerosol monitoring equipment, more samples per day can be collected and analyzed with the same minimum detectable concentrations as current systems. This work models hypothetical releases of 140 Ba and 131 I over a range of magnitudes corresponding to the inventory produced from the fission of about 100 g to 1 kiloton TNT-equivalent of 235 U. The releases occur over an entire year to incorporate the natural variability in atmospheric transport. Sampling equipment located at the 79 locations for radionuclide stations identified in the Comprehensive Nuclear-Test-Ban Treaty (CTBT) for the International Monitoring System are used to determine the detections of the individual releases. Alternative collection schemes in next generation equipment that collect 2, 3, or 4 samples per day, rather than the current 1 sample per day, would result in detections in many more samples at more stations with detections for a given release level. The authors posit that next generation equipment will result in increased network resilience to outages and improved source-location capability for lower yield source releases. The application of dual-detector and coincidence measurements to these systems would significantly boost sensitivity for some isotopes and would further enhance the monitoring capability.
Electrostatic dispersion can significantly impact the microphysical behavior of charged particles and ions until reaching zero space charge. However, although radioactive particles can be strongly charged in air, the influence of electrostatic dispersion has been neglected in understanding their behavior. This study is aimed at investigating the time evolution of the charge and size distributions of radioactive and nonradioactive particles in air and developing simple approaches for applications. With processes involving charging, aggregation, and electrostatic dispersion, a comprehensive population balance model (PBM) has been developed to examine particle charge/size distribution dynamics. It is shown that compared to nonradioactive particles, the charge and size distributions of radioactive particles may evolve differently with time because radioactivity and electrostatic dispersion can significantly affect the charging and aggregation kinetics of the particles. It is found that, after the Fukushima accident, background aerosols in the pathway of radioactive plumes might be highly charged due to ionizing radiation, suggesting that radiation fields may strongly influence in situ measurements of charged atmospheric particles. The comprehensive PBM is simplified, and then the verification and application of the simplified PBMs are discussed. This study provides useful insight into how radioactivity can affect the dynamic behavior of particles in atmospheric systems including radiation sources.
The key experimental and computational studies of the emission of long-lived radioactive fission products and actinides from uranium dioxide irradiated in BN-600 into sodium and the gas phase in the range 150–800°C, performed on the experimental bench at the Leipunskii Institute of Physics and Power Engineering, are presented. The results of measurements of the properties of aerosols of certain radioactive fission products formed upon heating of irradiated nuclear fuel in sodium are presented. The experimental results are of interest for evaluating the radiation impact of reactor facilities on workers and the public during beyond design basis accidents.
MACCS (MELCOR Accident Consequence Code System), WinMACCS, and MelMACCS now facilitate a multi-unit consequence analysis. MACCS evaluates the consequences of an atmospheric release of radioactive gases and aerosols into the atmosphere and is most commonly used to perform probabilistic safety assessments (PSAs) and related consequence analyses for nuclear power plants (NPPs). WinMACCS is a user-friendly preprocessor for MACCS. MelMACCS extracts source-term information from a MELCOR plot file. The current development can combine an arbitrary number of source terms, representing simultaneous releases from a multi-unit facility, into a single consequence analysis. The development supports different release signatures, fission product inventories, and accident initiation times for each unit. The treatment is completely general except that the model is currently limited to collocated units. A major practical consideration for performing a multi-unit PSA is that a comprehensive treatment for more than two units may involve an intractable number of combinations of source terms. This paper proposes and evaluates an approach for reducing the number of calculations to be tractable, even for sites with eight or ten units. The approximation error introduced by the approach is acceptable and is considerably less than other errors and uncertainties inherent in a Level 3 PSA.
The arterial blood PO(2) is increased in the prone position in animals and humans because of an improvement in ventilation (VA) and perfusion (Q) matching. However, the mechanism of improved VA/Q is unknown. This experiment measured regional VA/Q heterogeneity and the correlation between VA and Q in supine and prone positions in pigs. Eight ketamine-diazepam-anesthetized, mechanically ventilated pigs were studied in supine and prone positions in random order. Regional VA and Q were measured using fluorescent-labeled aerosols and radioactive-labeled microspheres, respectively. The lungs were dried at total lung capacity and cubed into 603-967 small ( approximately 1.7-cm(3)) pieces. In the prone position the homogeneity of the ventilation distribution increased (P = 0.030) and the correlation between VA and Q increased (correlation coefficient = 0.72 +/- 0.08 and 0.82 +/- 0.06 in supine and prone positions, respectively, P = 0.03). The homogeneity of the VA/Q distribution increased in the prone position (P = 0.028). We conclude that the improvement in VA/Q matching in the prone position is secondary to increased homogeneity of the VA distribution and increased correlation of regional VA and Q.
After Fukushima nuclear power plant accident at 2011, many counties decided to limit or hold operation and construction of nuclear power plant (NPP). Kori NPP unit-1, which was commissioned at 1978 and expected to operate until June 2017, was decided to stop its operation considering design life, political and public aspect in Korea while it was thought to be one of the reactors which had been affected by such nuclear accident. Accordingly, Korea Hydro and Nuclear Power Company, who is owner of Kori NPP unit-1, decided not to apply its life extension and is planning to prepare for the decommissioning. To establish decommissioning plan, it is needed to evaluate and secure the various safety factors including radiological safety. The biological shield has been neutron-activated by fission reaction during the operation of the reactor and various kinds of radionuclide including {sup 3}H, {sup 60}Co, {sup 55}Fe, and {sup 152}Eu are generated in the concrete. Thus, the biological shield dismantling worker will be exposed due to radiation from radioactive concrete and aerosol from its cutting. In this paper, the effective dose of the worker expected to dismantle biological shield is analyzed preliminarily. The dose assessment is analyzed on the external exposure from direct radiation and internal exposure due to inhalation and ingestion for the workers divided into three types.