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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.
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
3.
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
4.
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
5.
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
6.
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
7.
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
8.
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
9.
R. M. Ward S. R. F. Biegalski D. A. Haas W. Hennig 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):693-697
The monitoring of atmospheric radioxenon to ensure compliance with the Comprehensive Nuclear Test Ban Treaty (CTBT) has driven
the development of improved detectors for measuring xenon, including the development of a phoswich detector. This detector
uses only one PMT to detect β–γ coincidence, thus greatly reducing the bulk and electronics of the detector in comparison
to the ARSA-type detector. In this experiment, 135Xe was produced through neutron activation and a phoswich detector was used to attain spectra from the gas. These results
were compared to similar results from an ARSA-type β–γ coincidence spectrum. The spectral characteristics and resolution were
compared for the coincidence and beta spectra. Using these metrics, the overall performance of the phoswich detector for β–γ
coincidence of radioxenon was evaluated. 相似文献
10.
This paper presents the design and characterization of a prototype compact beta–gamma radioxenon detection system that utilizes a coplanar CdZnTe crystal, an array of SiPMs, and a plastic scintillator. The detector is directly mounted on a custom PCB. The system provides the advantage of room-temperature operation, while being compact, low noise, and with simple readout electronics. Preliminary measurements using 137Cs, 135Xe, and 133/133mXe were conducted to optimize various system parameters to achieve optimal resolution of key photopeaks. The purpose of this research was to explore the potential of these radiation detection elements for use in beta–gamma coincidence applications. 相似文献
11.
G. Le Petit A. Cagniant M. Morelle P. Gross P. Achim G. Douysset T. Taffary C. Moulin 《Journal of Radioanalytical and Nuclear Chemistry》2013,298(2):1159-1169
The verification regime of the comprehensive test ban treaty (CTBT) is based on a network of three different waveform technologies together with global monitoring of aerosols and noble gas in order to detect, locate and identify a nuclear weapon explosion down to 1 kt TNT equivalent. In case of a low intensity underground or underwater nuclear explosion, it appears that only radioactive gases, especially the noble gas which are difficult to contain, will allow identification of weak yield nuclear tests. Four radioactive xenon isotopes, 131mXe, 133mXe, 133Xe and 135Xe, are sufficiently produced in fission reactions and exhibit suitable half-lives and radiation emissions to be detected in atmosphere at low level far away from the release site. Four different monitoring CTBT systems, ARIX, ARSA, SAUNA, and SPALAX? have been developed in order to sample and to measure them with high sensitivity. The latest developed by the French Atomic Energy Commission (CEA) is likely to be drastically improved in detection sensitivity (especially for the metastable isotopes) through a higher sampling rate, when equipped with a new conversion electron (CE)/X-ray coincidence spectrometer. This new spectrometer is based on two combined detectors, both exhibiting very low radioactive background: a well-type NaI(Tl) detector for photon detection surrounding a gas cell equipped with two large passivated implanted planar silicon chips for electron detection. It is characterized by a low electron energy threshold and a much better energy resolution for the CE than those usually measured with the existing CTBT equipments. Furthermore, the compact geometry of the spectrometer provides high efficiency for X-ray and for CE associated to the decay modes of the four relevant radioxenons. The paper focus on the design of this new spectrometer and presents spectroscopic performances of a prototype based on recent results achieved from both radioactive xenon standards and air sample measurements. Major improvements in detection sensitivity have been reached and quantified, especially for metastable radioactive isotopes 131mXe and 133mXe with a gain in minimum detectable activity (about 2 × 10?3 Bq) relative to current CTBT SPALAX? system (air sampling frequency normalized to 8 h) of about 70 and 30 respectively. 相似文献
12.
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
13.
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
14.
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
15.
P. R. J. Saey A. Ringbom T. W. Bowyer M. Zähringer M. Auer A. Faanhof C. Labuschagne M. S. Al-Rashidi U. Tippawan B. Verboomen 《Journal of Radioanalytical and Nuclear Chemistry》2013,296(2):1133-1142
The Comprehensive Nuclear-Test-Ban Treaty (CTBT) specifies that radioxenon measurements should be performed at 40 or more stations worldwide within the International Monitoring System (IMS). Measuring radioxenon is one of the principle techniques to detect underground nuclear explosions. Specifically, presence and ratios of different radioxenon isotopes allows determining whether a detection event under consideration originated from a nuclear explosion or a civilian source. However, radioxenon monitoring on a global scale is a novel technology and the global civil background must be characterized sufficiently. This paper lays out a study, based on several unique measurement campaigns, of the worldwide concentrations and sources of verification relevant xenon isotopes. It complements the experience already gathered with radioxenon measurements within the CTBT IMS programme and focuses on locations in Belgium, Germany, Kuwait, Thailand and South Africa where very little information was available on ambient xenon levels or interesting sites offered opportunities to learn more about emissions from known sources. The findings corroborate the hypothesis that a few major radioxenon sources contribute in great part to the global radioxenon background. Additionally, the existence of independent sources of 131mXe (the daughter of 131I) has been demonstrated, which has some potential to bias the isotopic signature of signals from nuclear explosions. 相似文献
16.
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
17.
Alain Vivier Gilbert Le Petit Benoit Pigeon Xavier Blanchard 《Journal of Radioanalytical and Nuclear Chemistry》2009,282(3):743-748
When a net count value is below the type 1 error critical limit it is customary to declare that the activity is “below the
detection limit”. The content of this declaration is particularly impoverished, incapable for example of discriminating between
a net measurement just below the critical limit, but positive, and a negative net measurement, two types of information that
it is legitimate and intuitive to think do not have the same weight of information. In the case of a spectral measurement
of 131mXe and 133mXe certain information is available according to the various X and gamma emissions, which might all be below their respective
critical limits. We shall see that a Bayesian probabilistic approach can be used, without considering the critical limits,
to obtain anti-correlated maximum likelihood values taking all the information into account jointly and to obtain powerful
and pertinent information in the form of the absolute probability that the sample contains 131mXe and/or 133mXe, all possible activity values combined. Conversely, of course, this is used immediately to deduce the probability that
the sample does not contain 131mXe and/or 133mXe. This information enables the customary critical limit to be ignored. 相似文献
18.
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
19.
M. Tabasi M. Ghannadi-Maragheh l M. Shamsaii A. R. Khanchi 《Journal of Radioanalytical and Nuclear Chemistry》2005,264(3):679-686
Summary Separation and purification of 133Xe from acidic solution containing uranium, 99Mo and 131I has been developed. In the first step of this work, uranium pellets were dissolved under pressure (8-15 bar) in 8M nitric acid solution. Then133 Xe and other gases were conducted to activated charcoal cold trap. Final purification of 133Xe from impurities such as NOx, radioiodine and krypton was performed by passing through a molecular sieve preparative chromatographic column using helium as mobile phase. The final recovery of 133Xe from the separation-purification process was higher than 98%. Adsorption-desorption behavior of radioxenon on the charcoal and molecular sieves have also been studied and discussed. 相似文献
20.
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