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1.
Automated separation and measurement of radioxenon for the Comprehensive Test Ban Treaty 总被引:2,自引:0,他引:2
T. W. Bowyer K. H. Abel C. W. Hubbard A. D. McKinnon M. E. Panisko R. W. Perkins P. L. Reeder R. C. Thompson R. A. Warner 《Journal of Radioanalytical and Nuclear Chemistry》1998,235(1-2):77-82
A fully automatic radioxenon sampler/analyzer (ARSA) has been developed and demonstrated for the collection and quantitative
measurement of the four xenon radionuclides,131mXe(11.9 d),133mXe(2.2 d),133Xe(5.2 d), and135Xe(9.1 hr), in the atmosphere. These radionuclides are important signatures in monitoring for compliance to a Comprehensive
Test Ban Treaty (CTBT). Activity ratios of these radionuclides permit source attribution. Xenon, continuously and automatically
separated from the atmosphere, is automatically analyzed by electron-photon coincidence spectrometry providing a lower limit
of detection of about 100 μBq/m3. The demonstrated detection limit is about 100 times better than achievable with reported laboratory-based procedures for
the short-time collection intervals of interest. 相似文献
2.
P. L. Reeder T. W. Bowyer J. I. McIntyre W. K. Pitts 《Journal of Radioanalytical and Nuclear Chemistry》2001,248(3):617-622
The International Monitoring System for the Comprehensive Nuclear-Test-Ban Treaty will include measurements of Xe fission products. Pacific Northwest National Laboratory has developed an automated system for separating Xe from air which detects Xe fission products using a beta-gamma counting system for 131mXe, 133mXe, 133gXe, and 135gXe. Betas and conversion electrons are detected in a plastic scintillation cell containing the Xe sample. Gamma and X-rays are detected in a NaI(Tl) scintillation detector which surrounds the plastic scintillator sample cell. Two-dimensional pulse-height spectra of gamma-energy versus beta-energy are obtained. The plastic scintillator spectrum in coincidence with the 31-keV X-rays from 131mXe. 133mXe, and 133gXe is a complex mixture of conversion electrons and betas. A new technique to simultaneously measure the delayed coincidence (T
1/2 = 6.27 ns) between beta-particles from 133gXe and conversion electrons depopulating the 81-keV state in 133 Cs is being developed. This technique allows separation of the 133gXe beta spectrum from the conversion electrons due to 131mXe and 133mXe and uniquely quantifies all three nuclides. 相似文献
3.
W. Zhang K. Ungar I. Hoffman R. Lawrie 《Journal of Radioanalytical and Nuclear Chemistry》2009,280(1):121-128
To support interpretation of observed atmospheric 135Xe, 133Xe, 133mXe and 131mXe, a database of xenon radioisotope in the primary coolant of CANDU reactors has been established. This database is comprised
of 40000 records of high-quality xenon radioisotope analyses. Records from the database were retrieved by a specifically designed
data-mining module and subjected to further analysis. Results from the analysis were subsequently used to study isotopic ratios
of observed xenon radioisotopes in the CANDU reactor primary coolant. These studies provided novel and practical information
on the characterization of CANDU reactor xenon radioisotope releases, which can be used to discriminate between reactor effluence
and underground nuclear test releases. 相似文献
4.
Weihua Zhang Pawel Mekarski Jonathan Lam Kurt Ungar Eric Pellerin 《Journal of Radioanalytical and Nuclear Chemistry》2010,285(3):475-482
In this work, a Monte Carlo (MC) simulation model is established to accurately characterize a phoswich beta-gamma coincidence detector system. This model can be easily used to predict the beta-gamma coincidence efficiencies of xenon radioisotopes at various stable xenon concentrations in the counting cell. The results demonstrate that there is a significant inverse correlation between beta-gamma coincidence efficiency and stable xenon concentration. The influence of stable xenon concentration on beta-gamma coincidence counting efficiency has been investigated for each individual xenon radioisotope. The results indicate that the effect of stable xenon concentration on beta-gamma coincidence efficiency depends on the xenon radioisotope and its decay modes. The coincidence efficiency of 133Xe with 31.0-keV X-ray decay mode is the most affected one; and then followed by 131mXe, 133Xe with 81.0-keV gamma-ray decay mode, 133mXe and finally 135Xe. The study also indicates that the gamma absorption by xenon gas plays more of a role in the decrease of beta-gamma coincidence efficiency for 133Xe and 135Xe, and that the conversion electron spectrum shifting and broadening plays more of a role in the reduction of beta-gamma coincidence efficiency for the metastable radioxenon of 131mXe and 133mXe. 相似文献
5.
Georg Steinhauser Michael Lechermann Anders Axelsson Helmuth Böck Anders Ringbom Paul R. J. Saey Clemens Schlosser Mario Villa 《Journal of Radioanalytical and Nuclear Chemistry》2013,296(1):169-174
Radioxenon emissions of the TRIGA Mark II research reactor in Vienna were investigated with respect to a possible impact on the verification of the Comprehensive Nuclear Test-Ban-Treaty. Using the Swedish Automatic Unit for Noble Gas Acquisition (SAUNA II), five radioxenon isotopes 125Xe, 131mXe, 133mXe, 133Xe and 135Xe were detected, of which 125Xe is solely produced by neutron capture in stable atmospheric 124Xe and hence acts as an indicator for neutron activation processes. The other nuclides are produced in both fission and neutron capture reactions. The detected activity concentrations ranged from 0.0010 to 190 Bq/m³. The source of the radioxenon is not yet fully clarified, but it could be micro-cracks in the fuel cladding, fission of 235U contaminations on the outside of the fuel elements or neutron activation of atmospheric Xe. Neutron deficient 125Xe with its highly complex decay scheme was seen for the first time in a SAUNA system. In many experiments the activity ratios of the radioxenon nuclides carry the signature of nuclear explosions, if 131mXe is omitted. Only if 131mXe is included into the calculations of the isotopic activity ratios, the majority of the measurements revealed a “civil” signature (typical for a NPP). A significant contribution of the TRIGA Vienna to the global or European radioxenon inventory can be excluded. Due to the very low activities, the emissions are far below any concern for human health. 相似文献
6.
7.
D. A. Haas S. R. Biegalski K. M. Foltz Biegalski 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):677-680
The Spectral Deconvolution Analysis Tool (SDAT) software was developed to improve counting statistics and detection limits for nuclear explosion radionuclide measurements. SDAT utilizes spectral deconvolution spectroscopy techniques and can analyze both β–γ coincidence spectra for radioxenon isotopes and high-resolution HPGe spectra from aerosol monitors. The deconvolution algorithm of the SDAT requires a library of β–γ coincidence spectra of individual radioxenon isotopes to determine isotopic ratios in a sample. In order to get experimentally produced spectra of the individual isotopes, we have irradiated enriched samples of 130Xe, 132Xe, and 134Xe gas with a neutron beam from the TRIGA reactor at The University of Texas. The samples were counted in an Automated Radioxenon Sampler/Analyzer (ARSA) style β–γ coincidence detector. The spectra produced show that this method of radioxenon production yields samples with very high purity of the individual isotopes for 131mXe and 135Xe and a sample with a substantial 133mXe to 133Xe ratio. 相似文献
8.
M. Zähringer A. Becker M. Nikkinen P. Saey G. Wotawa 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):737-742
The Preparatory Commission of Comprehensive Nuclear Test-Ban-Treaty Organization is setting up a global network capable to
monitor treaty compliance. Specific monitoring systems and methodologies that match the needs of the International Monitoring
System (IMS), namely to clarify the nuclear character of suspect explosions, had to be developed for monitoring purposes during
the last decade. Four xenon isotopes, namely 133Xe, 135Xe, 133mXe and 131mXe play a key role here. A complex background from medical isotope production facilities and nuclear power plants, varying
over four orders of magnitude, challenges the system’s capability to distinguish these from treaty-relevant events. Available
measurement data are compared with model calculations. The importance of atmospheric transport modelling is demonstrated both
for completely understanding the civilian background and for explaining peak concentrations and abnormal events. New methodologies
for backtracking nuclide detections improved the capability to locate sources and corroborate the role of radioxenon monitoring. 相似文献
9.
Radioargon has been identified as a useful nuclide for verifying compliance with the Comprehensive Nuclear-Test-Ban Treaty. Use of 37Ar to identify a nuclear explosion requires quantification of contributions to the 37Ar background at a potential measurement site. A method of estimating 37Ar release activities using isotopes of radioxenon and radioargon has been developed in this paper. Numerical solutions to the system of equations describing air-activation in a reactor were used to determine ratios of release activities for 135Xe/133Xe, 133mXe/131mXe, and 37Ar /41Ar as function of irradiation time and off-gas residence time prior to measurement and release. Published radioactive noble gas effluent data for the High Flux Isotope Reactor, HFIR (ORNL) from the year 1996 to 2010 were compiled as a test data set to predict the 37Ar release on a yearly basis. An average 37Ar release rate of 1.86 × 1010 Bq per year was calculated. The estimated release rate was used as a source term for atmospheric transport to run a test case for 37Ar release over a typical HFIR operation cycle. Results showed that ground-level concentrations of 37Ar did not exceed the minimum detectable concentration for a 37Ar field measurement system beyond the immediate vicinity of the release point. 相似文献
10.
Martin E. Keillor Matthew W. Cooper James C. Hayes Justin I. McIntyre 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):699-702
Pacific Northwest National Laboratory uses beta-gamma coincidence detectors in a number of xenon sampling and measurement
systems to enable simultaneous, sensitive measurements of 131Xe, 133Xe, 133mXe, and 135Xe for treaty monitoring applications. In recent years, a new style of beta–gamma detector was developed to improve upon the
detector module used in the Automated Radioxenon Sampler/Analyzer. The results of an MCNP5 Monte Carlo simulation of the new
detector cell are presented, with particular emphasis on the identification of an energy deposition sequence with the potential
to introduce significant error into the detector efficiency calibration. This sequence occurs when an 81 keV gamma from 133Xe is absorbed in an inactive region of the CsI(Na) scintillator, followed by emission of a 31 keV X-ray from cesium (or possibly
a 28.5 keV X-ray from iodine). These X-rays add excess counts into the 31 keV peak observed in the decay of 133Xe. The impact of this effect on different efficiency calibration techniques is discussed. 相似文献
11.
Troy A. Robinson Nick R. Mann Christopher P. Oertel Matthew G. Watrous Christopher A. McGrath John P. Peterson 《Journal of Radioanalytical and Nuclear Chemistry》2017,311(3):1681-1686
Quantification of low-activity noble gases in air is typically accomplished through separation of the noble gas from air followed by radiometric assay. This work is aimed at quantification of radioactive noble gas in air without extraction. A high pressure aluminum Marinelli counting vessel was designed and fabricated that can be placed on a coaxial high purity germanium detector for gamma counting. Characterization of the performance of this Marinelli using MCNP modeling, large excesses of activity, and low-activity noble gas in air is discussed. Minimum detectable concentrations achieved during a 24 h count are: 5, 10, 50, and 1 Bq/m3 for 133Xe, 133mXe, 131mXe, and 135Xe, respectively. 相似文献
12.
E. Nava A. Rizzo R. Lorenzelli S. Salvi P. Bartolomei F. Padoani 《Journal of Radioanalytical and Nuclear Chemistry》2013,296(2):1163-1167
The strategic value of noble gas capability has been recently recognized by ENEA for the acquisition of data about anthropogenic activities. Within the framework of institutional agreements, a laboratory for measurement of radioactive noble gases is under construction for environmental analysis and for monitoring studies in connection with issues related to the nuclear fuel cycle to distinguish the anthropogenic contributions to the environment. This research is intended to contribute also to the international effort to support the comprehensive nuclear-test-ban treaty verification capability. The present work summarizes the status of implementation of the noble gas laboratory at the ENEA Brasimone research centre that is located in the north-centre part of Italy by the Brasimone lake at about 850 m altitude. The radionuclides of interest are the following four xenon radioisotopes: 131mXe, 133mXe, 133Xe and 135Xe. The noble gas system under development at ENEA has three separate components: air collection (sampling and adsorption), processing (gas extraction and purification) and measurement (gamma-ray spectrometry analysis). The separation of the sampling equipment from the analysis is seen as necessary for the effectiveness of extensive sampling campaigns, as required in monitoring programs. Refurbishment is currently under way to accommodate a more sensitive acquisition system. 相似文献
13.
D. A. Haas S. R. Biegalski K. M. Foltz Biegalski 《Journal of Radioanalytical and Nuclear Chemistry》2008,277(3):561-565
In support of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), improvements have been made to the model of the Automated
Radioxenon Sampler/Analyzer (ARSA) β-γ coincidence detector for radioxenon monitoring. MCNPX is used to simulate the detector
response for all the electrons and photons emitted from 131mXe, 133Xe, 133mXe, 135Xe, and 137Cs signals. A MatLab code was written to incorporate the MCNPX results in the calculation of β-γ coincidence spectra. These
will aid in the development of the Spectral Deconvolution Analysis Tool (SDAT)1 and to calibrate β-γ coincidence systems. The models developed for this work include improvements over previous models in
their ability to address Compton scattering in the β-cell, and the β-distribution offset in the 31 keV γ-ray region for 133Xe. 相似文献
14.
Y. Jao W. L. Cheng H. J. Chen C. C. Shaeh C. C. Huang Y. M. Lin 《Journal of Radioanalytical and Nuclear Chemistry》1995,194(2):411-417
This study was performed under the joint TRMC/INER program for the determination of low level85Kr and133Xe concentrations in the environmental air samples. Based on cryogenic adsorption of krypton and xenon on charcoal followed by chromatographic separation from other gases, the85Kr and133Xe recovered from 200 liters of atmospheric air can be determined by either on-line gas flow proportional counter or liquid scintillation counting. The recovery yields of krypton and xenon examined by using85Kr and133Xe tracers were nearly 100%. The minimum detectable activity of85Kr and133Xe by gas flow proportional counting is about 7.40 Bq. The method is satisfactory for environmental monitoring applications under abnormal conditions of nuclear facilities. However, for lower level environmental85Kr and133Xe measurements, the liquid scintillation counting method can be applied due to their extremely low detection limits (i.e. 0.107 Bq and 0.093 Bq for85Kr and133Xe, respectively). Using this method, the measurable limits of concentrations are 0.535 Bq/m3 and 0.466 Bq/m3 for85Kr and133Xe, respectively. 相似文献
15.
S. Biegalski A. Flory D. Haas J. Ely M. Cooper 《Journal of Radioanalytical and Nuclear Chemistry》2013,296(1):471-476
The standard deconvolution analysis tool (SDAT) was developed for analysis of radioxenon β–γ coincidence spectra measured as part of the international monitoring system as defined in the comprehensive nuclear-test-ban treaty. The SDAT software analyzes each β–γ coincidence spectrum by fitting library vectors of each radionuclide of interest: 131mXe, 133mXe, 133Xe, and 135Xe. Detector background and radon are incorporated as optional components of the sample solution. Results are reported in mBq m?3. A new graphical user interface has been developed to facilitate ease of use and improve the data visualization. Automated energy versus channel calibration algorithms were developed and implemented based on 137Cs β–γ coincidence spectra. Details on the user tool and testing are included. 相似文献
16.
S. R. Biegalski T. Saller J. Helfand K. M. F. Biegalski 《Journal of Radioanalytical and Nuclear Chemistry》2010,284(3):663-668
As part of the Comprehensive Nuclear Test-Ban Treaty (CTBT), the International Monitoring System (IMS) was established to
monitor the world for nuclear weapon explosions. As part of this network, systems are in place to monitor the atmosphere for
radioxenon. The IMS routinely detects radioxenon from sources other than nuclear explosions. One of these radioxenon sources
is radiopharmaceutical production facilities. This is a sensitivity study on the nuclear forensic signals possible from such
facilities. A fission process model was produced to calculate the activity of 131mXe, 133mXe, 133Xe and 135Xe in the process utilized to produce 99Mo and 131I for medical applications through high enriched uranium fission. The computer model accounts for fractionation of radionuclides
within a decay chain that may result from filtering or chemical procedures. Ratios of the radioxenon isotopes are calculated
as a function of decay time after the release. The ratios are then compared to those expected from nuclear explosions. The
main conclusion from this work is that the two main factors that affect the nuclear forensic signal from radiopharmaceutical
production facilities are the sample irradiation time and the use of emission gas storage tanks. 相似文献
17.
T. W. Bowyer K. H. Abel C. W. Hubbard M. E. Panisko P. L. Reeder R. C. Thompson R. A. Warner 《Journal of Radioanalytical and Nuclear Chemistry》1999,240(1):109-122
Pacific Northwest National Laboratory, with guidance and support from the U.S. Department of Energy's NN-20 Comprehensive
Test Ban Treaty (CTBT) Research and Development program, has developed and demonstrated a fully automatic sampler-analyzer
(ARSA) for the collection and quantitative measurement of the four xenon radionuclides,131mXe (11.9 d),133mXe (2.19 d),133Xe (5.24 d), and135Xe (9.10 h), in the atmosphere. These radionuclides are important signatures in monitoring for compliance to a CTBT, and may
have applications in stack monitoring and other areas where xenon radionuclides are present. The activity ratios between certain
of these radionuclides permit discrimination between radioxenon originating from nuclear detonations and that from nuclear
reactor operations, nuclear fuel reprocessing, or from medical isotope production and usage. With the ARSA system, xenon is
continuously and automatically separated from the atmosphere at flow rates of about 100 lpm by sorption-bed techniques. Samples
collected in 8 hours are automatically analyzed by electron-photon coincidence spectrometry to provide detection sensitivities
as low as 100 μBq/m3 of air. This sensitivity is about 10-fold better than achieved with reported laboratory-based procedures1 for the short time collection intervals of interest. Gamma-ray energy spectra and gas analysis data are automatically collected. 相似文献
18.
P. L. Reeder T. W. Bowyer R. W. Perkins 《Journal of Radioanalytical and Nuclear Chemistry》1998,235(1-2):89-94
A beta-gamma coincidence counting system has been developed for automated analysis of Xe gas samples separated from air. The
Xe gas samples are contained in a cylindrical plastic scintillator cell located between two NaI(T1) scintillation detectors.
The X-ray and gamma spectra gated by coincident events in the plastic scintillator cell are recorded for each NaI(T1) crystal.
The characteristic signatures of the131mXe,133gXe,133mXe, and135gXe isotopes of interest for nuclear test-ban verification as well as the procedures and results of absolute efficiency measurements
are described. A NaI(T1) crystal with provision for 4 sample cells has been implemented for the system to be deployed in the
field. Examples of data on ambient air samples in New York City obtained with the field prototype are presented. 相似文献
19.
Justin I. McIntyre Mathew Cooper April J. Carman Theodore W. Bowyer Anthony Day Derek Haas James C. Hayes Tom R. Heimbigner Charlie Hubbard Kevin Litke Michael Ripplinger Brian Schrom Reynold Suarez 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):755-759
Absolute efficiency calibration of radiometric detectors is frequently difficult and requires careful detector modeling and accurate knowledge of the radioactive source used. In the past we have calibrated the β–γ coincidence detector of the Automated Radioxenon Sampler/Analyzer (ARSA) using a variety of sources and techniques which have proven to be less than desirable (Reeder et al., J Radioanal Nucl Chem, 235, 1989). A superior technique has been developed that uses the conversion-electron (CE) and X-ray coincidence of 131mXe to provide a more accurate absolute gamma efficiency of the detector. The 131mXe is injected directly into the beta cell of the coincident counting system and no knowledge of absolute source strength is required. In addition, 133Xe is used to provide a second independent means to obtain the absolute efficiency calibration. These two data points provide the necessary information for calculating the detector efficiency and can be used in conjunction with other noble gas isotopes to completely characterize and calibrate the ARSA nuclear detector. In this paper we discuss the techniques and results that we have obtained. 相似文献
20.
J. C. Hayes T. W. Bowyer E. A. Cordova R. R. Kirkham A. Misner K. B. Olsen V. T. Woods Dudley Emer 《Journal of Radioanalytical and Nuclear Chemistry》2013,296(2):869-876
It is well known that radon is present in relatively high concentrations below the surface of the Earth due to natural decay of uranium and thorium. However, less information is available on the background levels of other isotopes such as 133Xe and 131mXe produced via spontaneous fission of either manmade or naturally occurring elements. The background concentrations of radioxenon in the subsurface are important to understand because these isotopes potentially can be used to confirm violations of the comprehensive nuclear-test-ban treaty during an on-site inspection. Recently, Pacific Northwest National Laboratory measured radioxenon concentrations from the subsurface at the Nevada Nuclear Security Site (NNSS—formerly known as the Nevada Test Site) to determine whether xenon isotope background levels could be detected from spontaneous fission of naturally occurring uranium or legacy 240Pu as a result of historic nuclear testing. In this paper, we discuss the results of those measurements and review the sources of xenon background that must be taken into account during OSI noble gas measurements. 相似文献