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Title: Detection in subsurface air of radioxenon released from medical isotope production

Abstract

Abstract Under the Comprehensive Nuclear-Test-Ban Treaty, an On-Site Inspection (OSI) may be conducted to clarify whether a nuclear explosion has been carried out in violation of Article I of the Treaty. A major component of an OSI is the measurement of subsurface gases in order to detect radioactive noble gases that are produced in a nuclear explosion, particularly radioxenon and radioargon. In order to better understand potential backgrounds of these gases, a sampling campaign was performed near Canadian Nuclear Laboratories in the Ottawa River Valley, a major source of environmental radioxenon. First of their kind measurements of atmospheric radioxenon imprinted into the shallow subsurface from an atmospheric pressure driven force were made using current OSI techniques to measure both atmospheric and subsurface gas samples which were analyzed for radioxenon. These measurements indicate that under specific sampling conditions, on the order of one percent of the atmospheric radioxenon concentration may be measured via subsurface sampling.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1344035
Report Number(s):
PNNL-SA-117917
Journal ID: ISSN 0265-931X; 453060036
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Environmental Radioactivity; Journal Volume: 167; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
07 ISOTOPE AND RADIATION SOURCES

Citation Formats

Johnson, Christine, Biegalski, Steven, Haas, Derek, Lowrey, Justin, Bowyer, Theodore, Hayes, James, Suarez, Reynold, and Ripplinger, Michael. Detection in subsurface air of radioxenon released from medical isotope production. United States: N. p., 2017. Web. doi:10.1016/j.jenvrad.2016.10.021.
Johnson, Christine, Biegalski, Steven, Haas, Derek, Lowrey, Justin, Bowyer, Theodore, Hayes, James, Suarez, Reynold, & Ripplinger, Michael. Detection in subsurface air of radioxenon released from medical isotope production. United States. doi:10.1016/j.jenvrad.2016.10.021.
Johnson, Christine, Biegalski, Steven, Haas, Derek, Lowrey, Justin, Bowyer, Theodore, Hayes, James, Suarez, Reynold, and Ripplinger, Michael. Wed . "Detection in subsurface air of radioxenon released from medical isotope production". United States. doi:10.1016/j.jenvrad.2016.10.021.
@article{osti_1344035,
title = {Detection in subsurface air of radioxenon released from medical isotope production},
author = {Johnson, Christine and Biegalski, Steven and Haas, Derek and Lowrey, Justin and Bowyer, Theodore and Hayes, James and Suarez, Reynold and Ripplinger, Michael},
abstractNote = {Abstract Under the Comprehensive Nuclear-Test-Ban Treaty, an On-Site Inspection (OSI) may be conducted to clarify whether a nuclear explosion has been carried out in violation of Article I of the Treaty. A major component of an OSI is the measurement of subsurface gases in order to detect radioactive noble gases that are produced in a nuclear explosion, particularly radioxenon and radioargon. In order to better understand potential backgrounds of these gases, a sampling campaign was performed near Canadian Nuclear Laboratories in the Ottawa River Valley, a major source of environmental radioxenon. First of their kind measurements of atmospheric radioxenon imprinted into the shallow subsurface from an atmospheric pressure driven force were made using current OSI techniques to measure both atmospheric and subsurface gas samples which were analyzed for radioxenon. These measurements indicate that under specific sampling conditions, on the order of one percent of the atmospheric radioxenon concentration may be measured via subsurface sampling.},
doi = {10.1016/j.jenvrad.2016.10.021},
journal = {Journal of Environmental Radioactivity},
number = C,
volume = 167,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}
  • Abstract The International Monitoring System (IMS) of the Comprehensive-Nuclear-Test-Ban-Treaty monitors the atmosphere for radioactive xenon leaking from underground nuclear explosions. Emissions from medical isotope production represent a challenging background signal when determining whether measured radioxenon in the atmosphere is associated with a nuclear explosion prohibited by the treaty. The Australian Nuclear Science and Technology Organisation (ANSTO) operates a reactor and medical isotope production facility in Lucas Heights, Australia. This study uses two years of release data from the ANSTO medical isotope production facility and Xe-133 data from three IMS sampling locations to estimate the annual releases of Xe-133 from medicalmore » isotope production facilities in Argentina, South Africa, and Indonesia. Atmospheric dilution factors derived from a global atmospheric transport model were used in an optimization scheme to estimate annual release values by facility. The annual releases of about 6.8×1014 Bq from the ANSTO medical isotope production facility are in good agreement with the sampled concentrations at these three IMS sampling locations. Annual release estimates for the facility in South Africa vary from 1.2×1016 to 2.5×1016 Bq and estimates for the facility in Indonesia vary from 6.1×1013 to 3.6×1014 Bq. Although some releases from the facility in Argentina may reach these IMS sampling locations, the solution to the objective function is insensitive to the magnitude of those releases.« less
  • Abstract Batan Teknologi (BaTek) operates an isotope production facility in Serpong, Indonesia that supplies 99mTc for use in medical procedures. Atmospheric releases of Xe-133 in the production process at BaTek are known to influence the measurements taken at the closest stations of the International Monitoring System (IMS). The purpose of the IMS is to detect evidence of nuclear explosions, including atmospheric releases of radionuclides. The xenon isotopes released from BaTek are the same as those produced in a nuclear explosion, but the isotopic ratios are different. Knowledge of the magnitude of releases from the isotope production facility helps inform analystsmore » trying to decide whether a specific measurement result came from a nuclear explosion. A stack monitor deployed at BaTek in 2013 measured releases to the atmosphere for several isotopes. The facility operates on a weekly cycle, and the stack data for June 15-21, 2013 show a release of 1.84E13 Bq of Xe-133. Concentrations of Xe-133 in the air are available at the same time from a xenon sampler located 14 km from BaTek. An optimization process using atmospheric transport modeling and the sampler air concentrations produced a release estimate of 1.88E13 Bq. The same optimization process yielded a release estimate of 1.70E13 Bq for a different week in 2012. The stack release value and the two optimized estimates are all within 10 percent of each other. Weekly release estimates of 1.8E13 Bq and a 40 percent facility operation rate yields a rough annual release estimate of 3.7E13 Bq of Xe-133. This value is consistent with previously published estimates of annual releases for this facility, which are based on measurements at three IMS stations. These multiple lines of evidence cross-validate the stack release estimates and the release estimates from atmospheric samplers.« less
  • After performing a first multi-model exercise in 2015 a comprehensive and technically more demanding atmospheric transport modelling challenge was organized in 2016. Release data were provided by the Australian Nuclear Science and Technology Organization radiopharmaceutical facility in Sydney (Australia) for a one month period. Measured samples for the same time frame were gathered from six International Monitoring System stations in the Southern Hemisphere with distances to the source ranging between 680 (Melbourne) and about 17,000 km (Tristan da Cunha). Participants were prompted to work with unit emissions in pre-defined emission intervals (daily, half-daily, 3-hourly and hourly emission segment lengths) andmore » in order to perform a blind test actual emission values were not provided to them. Despite the quite different settings of the two atmospheric transport modelling challenges there is common evidence that for long-range atmospheric transport using temporally highly resolved emissions and highly space-resolved meteorological input fields has no significant advantage compared to using lower resolved ones. As well an uncertainty of up to 20% in the daily stack emission data turns out to be acceptable for the purpose of a study like this. Model performance at individual stations is quite diverse depending largely on successfully capturing boundary layer processes. No single model-meteorology combination performs best for all stations. Moreover, the stations statistics do not depend on the distance between the source and the individual stations. Finally, it became more evident how future exercises need to be designed. Set-up parameters like the meteorological driver or the output grid resolution should be pre-scribed in order to enhance diversity as well as comparability among model runs.« less
  • Fission gases such as 133Xe are used extensively for monitoring the world for signs of nuclear testing in systems such as the International Monitoring System (IMS). These gases are also produced by nuclear reactors and by fission production of 99Mo for medical use. Recently, medical isotope production facilities have been identified as the major contributor to the background of radioactive xenon isotopes (radioxenon) in the atmosphere (Saey, et al., 2009). These releases pose a potential future problem for monitoring nuclear explosions if not addressed. As a starting point, a maximum acceptable daily xenon emission rate was calculated, that is bothmore » scientifically defendable as not adversely affecting the IMS, but also consistent with what is possible to achieve in an operational environment. This study concludes that an emission of 5×109 Bq/day from a medical isotope production facility would be both an acceptable upper limit from the perspective of minimal impact to monitoring stations, but also appears to be an achievable limit for large isotope producers.« less
  • Abstract The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward (Bowyer et al., 2013). Fission-based production of 99Mo for medical purposes also releases radioxenon isotopes to the atmosphere (Saey, 2009). One of the ways to mitigate the effect of emissions from medical isotope production is the use of stack monitoring data, if it were available, so thatmore » the effect of radioactive xenon emissions could be subtracted from the effect from a presumed nuclear explosion, when detected at an IMS station location. To date, no studies have addressed the impacts the time resolution or data accuracy of stack monitoring data have on predicted concentrations at an IMS station location. Recently, participants from seven nations used atmospheric transport modeling to predict the time-history of 133Xe concentration measurements at an IMS station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well (a high composite statistical model comparison rank or a small mean square error with the measured values). The results suggest release data on a 15 min time spacing is best. The model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. Further research is needed to identify optimal methods for selecting ensemble members and those methods may depend on the specific transport problem. None of the submissions based only on the stack monitoring data predicted the small measured concentrations very well. The one submission that best predicted small concentrations also included releases from nuclear power plants. Modeling of sources by other nuclear facilities with smaller releases than medical isotope production facilities may be important in discriminating those releases from releases from a nuclear explosion.« less