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1.
A global monitoring system for atmospheric radioactivity is being established as part of the International Monitoring System that will verify compliance with the comprehensive nuclear-test-ban treaty (CTBT) once the treaty has entered into force. This paper studies isotopic activity ratios to support the interpretation of observed atmospheric concentrations of 135I, 133I and 131I. The goal is to distinguish nuclear explosion sources from civilian releases. Simulated nuclear explosion releases along with observational data of radioiodine releases from historic nuclear explosions at the Nevada Test Site are compared to simulated light water reactor releases in order to provide a proof of concept for source discrimination based on radioiodine isotopic activity ratios.  相似文献   

2.
A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System that will verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT) once the treaty has entered into force. This paper studies isotopic activity ratios to support the interpretation of observed atmospheric concentrations of 135Xe, 133mXe, 133Xe and 131mXe. The goal is to distinguish nuclear explosion sources from civilian releases. Simulations of nuclear explosions and reactors, empirical data for both test and reactor releases as well as observations by measurement stations of the International Noble Gas Experiment (INGE) are used to provide a proof of concept for the isotopic ratio based method for source discrimination.  相似文献   

3.
During on-site inspections to verify the comprehensive nuclear-test-ban treaty (CTBT), soil gas samples may be taken and analysed for their content of the xenon isotopes 131mXe, 133Xe, 133mXe and 135Xe in order to identify a suspected underground nuclear test. These samples might contain natural radioxenon which is present as a trace gas in the ground. This work analyses the different production mechanisms of natural lithospheric radioxenon to assess theoretically the background concentration under different sampling conditions. The results imply that the equilibrium concentrations of the examined xenon isotopes can be measured in certain rock types using actual CTBTO on-site inspection equipment. Radioxenon production is dominated by spontaneous fission of 238U, resulting in a reactor-like xenon isotopic signature rather than an explosion-like signature.  相似文献   

4.
Activity concentration data from ambient radioxenon measurements in ground level air, which were carried out in Europe in the framework of the International Noble Gas Experiment (INGE) in support of the development and build-up of a radioxenon monitoring network for the Comprehensive Nuclear-Test-Ban Treaty verification regime are presented and discussed. Six measurement stations provided data from 5 years of measurements performed between 2003 and 2008: Longyearbyen (Spitsbergen, Norway), Stockholm (Sweden), Dubna (Russian Federation), Schauinsland Mountain (Germany), Bruyères-le-Châtel and Marseille (both France). The noble gas systems used within the INGE are designed to continuously measure low concentrations of the four radioxenon isotopes which are most relevant for detection of nuclear explosions: 131mXe, 133mXe, 133Xe and 135Xe with a time resolution less than or equal to 24 h and a minimum detectable concentration of 133Xe less than 1 mBq/m3. This European cluster of six stations is particularly interesting because it is highly influenced by a high density of nuclear power reactors and some radiopharmaceutical production facilities. The activity concentrations at the European INGE stations are studied to characterise the influence of civilian releases, to be able to distinguish them from possible nuclear explosions. It was found that the mean activity concentration of the most frequently detected isotope, 133Xe, was 5–20 mBq/m3 within Central Europe where most nuclear installations are situated (Bruyères-le-Châtel and Schauinsland), 1.4–2.4 mBq/m3 just outside that region (Stockholm, Dubna and Marseille) and 0.2 mBq/m3 in the remote polar station of Spitsbergen. No seasonal trends could be observed from the data. Two interesting events have been examined and their source regions have been identified using atmospheric backtracking methods that deploy Lagrangian particle dispersion modelling and inversion techniques. The results are consistent with known releases of a radiopharmaceutical facility.  相似文献   

5.
Atmospheric measurement of radioactive xenon isotopes (radioxenon) plays a key role in remote monitoring of nuclear explosions, since it has a high capability to capture radioactive debris for a wide range of explosion scenarios. It is therefore a powerful tool in providing evidence for nuclear testing, and is one of the key components of the verification regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The reliability of this method is largely based on a well-developed measurement technology. In the 1990s, with the prospect of the build-up of a monitoring network for the CTBT, new development of radioxenon equipment started. This article summarizes the physical and technical principles upon which the radioxenon technology is based and the advances the technology has undergone during the last 10 years. In contrast to previously used equipment, which was manually operated, the new generation of radioxenon monitoring equipment is designed for automated and continuous operation in remote field locations. Also the analytical capabilities of the equipment were strongly enhanced. Minimum detectable concentrations of the recently developed systems are well below 1 mBq/m3 for the key nuclide 133Xe for sampling periods between 8 and 24 h. All the systems described here are also able to separately measure with low detection limits the radioxenon isotopes 131mXe, 133mXe and 135Xe, which are also relevant for the detection of nuclear tests. The equipment has been extensively tested during recent years by operation in a laboratory environment and in field locations, by performing comparison measurements with laboratory type equipment and by parallel operation. These tests demonstrate that the equipment has reached a sufficiently high technical standard for deployment in the global CTBT verification regime.  相似文献   

6.
The value of the 133Xe/133mXe isometric activity ratio for the stationary regime of reactor work is about 35, and that for an instant fission (explosion) is about 11, which allowed estimation of the nuclear component of the instant (explosion) energy release during the NPP accident. Atmospheric xenon samples were taken at the trajectory of accident product transfers (in the Cherepovetz area); these samples were measured by a gamma spectrometer, and the 133Xe/133mXe ratio was determined as an average value of 22.4. For estimations a mathematic model was elaborated considering both the value of instant released energy and the schedule of reactor power change before the accident, as well as different fractionation conditions on the isobaric chain. Comparison of estimated results with the experimental data showed the value of the instant specific energy release in the Chernobyl NPP accident to be 2·105–2·106 J/Wt or 6·1014–6·1015 J (100–1,000 kt). This result is matched up to a total reactor power of 3,200 MWt. However this estimate is not comparable with the actual explosion scale estimated as 10t TNT. This suggests a local character of the instant nuclear energy release and makes it possible to estimate the mass of fuel involved in this explosion process to be from 0.01 to 0.1% of total quantity.  相似文献   

7.
The announced October 2006 nuclear test explosion in the Democratic People’s Republic of Korea (DPRK) has been the first real test regarding the technical capabilities of the verification system built up by the Vienna-based Provisional Technical Secretariat (PTS) of the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) to detect and locate a nuclear test event. This paper enhances the resolution of the DPRK events’ xenon source reconstruction published by Saey et al. (2007, “A long distance measurement of radioxenon in Yellowknife, Canada, in late October 2006”, GRL, Vol. 34, L20802) that was based solely on radio-xenon measurements taken at the remote radionuclide station in Yellowknife, Canada by involving additional measurements taken by a mobile noble gas system deployed quite close to the event location in the Republic of Korea (ROK). Moreover the horizontal resolution of the forward and backward atmospheric transport modelling methods applied for the source scenario reconstruction has been enhanced appropriately to reflect the considerably shorter source-receptor distances examined in comparison to the previously published source reconstruction. It is shown that the 133Xe measurements in Yellowknife could register 133Xe traces from the nuclear explosion during the first 3 days after the event, while the mobile measurements were rather sensitive to releases during days 2–4 after the explosion. According to the analysis, the most likely source scenario would consist of an initial (possibly up to 21 h delayed) venting of 1 × 10?15 Bq 133Xe during the first 24 h, followed by a two orders of magnitude weaker seepage during the following 3 days. Both measurements corroborate the scenario of a rather rapid venting and soil diffusion of the 133Xe yielded during the explosion. While the Swedish mobile measurements were crucial to enhancement of the reconstruction of the source scenario, given the installation status of the IMS xenon network at the time of the event, a sensitivity analysis revealed that the fully developed network would have been able to detect 133Xe traces from the Korean explosion at a number of stations and allowed for an even better constraint on the release function. The station Ussuriysk, Russia, being in operation in 2006, would have registered 133Xe within 1 day and with a three orders of magnitudes stronger signal compared to the detection at Yellowknife.  相似文献   

8.
Detonation gases released by an underground nuclear test include trace amounts of 133Xe and 37Ar. In the context of the Comprehensive Nuclear Test Ban Treaty, On Site Inspection Protocol, such gases released from or sampled at the soil surface could be used to indicate the occurrence of an explosion in violation of the treaty. To better estimate the levels of detectability from an underground nuclear test (UNE), we developed mathematical models to evaluate the processes of 133Xe and 37Ar transport in fractured rock. Two models are developed respectively for representing thermal and isothermal transport. When the thermal process becomes minor under the condition of low temperature and low liquid saturation, the subsurface system is described using an isothermal and single-gas-phase transport model and barometric pumping becomes the major driving force to deliver 133Xe and 37Ar to the ground surface. A thermal test is simulated using a nonisothermal and two-phase transport model. In the model, steam production and bubble expansion are the major processes driving noble gas components to ground surface. After the temperature in the chimney drops below boiling, barometric pumping takes over the role as the major transport process.  相似文献   

9.
Monitoring of Xe and Kr radionuclides was conducted from August 2006 to 30 July 2008 within the framework of ISTC Project #2133. Cherepovets City in Vologda Province and St. Petersburg were chosen as monitoring locations. Kr–Xe concentrate samples were obtained as a result of processing of several thousand m3 of atmospheric air. New results of 85Kr monitoring show, that for last 15 years, the 85Kr volumetric activity in the atmospheric air of the northwest region of Russia has increased approximately 50% and has achieved a level of 1.5 Bq/m3. This value correlates well with similar data for Western Europe and Japan. The xenon fraction (80–160 cm3 under STP) is adsorbed on charcoal in the ampoule, which is measured in the well of HPGe gamma detector. Minimum detectable concentration (MDC) of 133Xe for this technique is 0.008 mBq/m3, and it is the most sensitive method used today. The 133Xe concentration in the atmospheric air of Cherepovets City varied in the monitoring period ranging from 0.09 to 2.5 mBq/m3. During the period of March 2007–30 July 2008, 133Xe activity concentration in the atmospheric air of St. Petersburg changed from background values (0.2–0.3 mBq/m3) to 185 mBq/m3 and for approximately 20% of the samples 135Xe was also measured with the 135Xe/133Xe activity ratio varied within the range of 0.03–3.5.  相似文献   

10.
The present part of the publication (Part II) deals with long range dispersion of radionuclides emitted into the atmosphere during the Fukushima Dai-ichi accident that occurred after the March 11, 2011 tsunami. The first part (Part I) is dedicated to the accident features relying on radionuclide detections performed by monitoring stations of the Comprehensive Nuclear Test Ban Treaty Organization network. In this study, the emissions of the three fission products Cs-137, I-131 and Xe-133 are investigated. Regarding Xe-133, the total release is estimated to be of the order of 6 × 1018 Bq emitted during the explosions of units 1, 2 and 3. The total source term estimated gives a fraction of core inventory of about 8 × 1018 Bq at the time of reactors shutdown. This result suggests that at least 80 % of the core inventory has been released into the atmosphere and indicates a broad meltdown of reactor cores. Total atmospheric releases of Cs-137 and I-131 aerosols are estimated to be 1016 and 1017 Bq, respectively. By neglecting gas/particulate conversion phenomena, the total release of I-131 (gas + aerosol) could be estimated to be 4 × 1017 Bq. Atmospheric transport simulations suggest that the main air emissions have occurred during the events of March 14, 2011 (UTC) and that no major release occurred after March 23. The radioactivity emitted into the atmosphere could represent 10 % of the Chernobyl accident releases for I-131 and Cs-137.  相似文献   

11.
Cores and coats of five coated diamonds, one from Botswana and four from Zaire, were separately analyzed for their noble gases. Noble gases in the diamonds are essentially of a trapped origin, including radio- and nucleogenic components such as4He, 40Ar, 21Neexcess and excesses in Xe isotopes (129, 131–136). The fairly precise elemental and isotopic abundances allow us to infer the noble gas state in the ancient mantle. 20Ne/22Ne ratios are fairly constant (11.8 ± 0.4), and very close to that of SEP (solar energetic particle)-Ne, but distinctly different from the atmospheric ratio. 21Ne/22Ne ratios range from 0.028 to 0.06, which is attributed to nucleogenic 21Ne from 18O(α, n)21Ne and 24Mg(n, α)21Ne reactions. The difference in 20Ne/22Ne between atmosphere and mantle can be attributed to the hydrodynamic escape of hydrogen from the primitive atmosphere during the very early stage in the Earth's history. 38Ar/36Ar and Kr isotopic ratios are identical to the atmospheric values within 1%. After correction for 238U- or 244Pu-fission Xe, the 131–136Xe abundance ratios are indistinguishable from atmospheric ratios. Lighter Xe isotopes (124–128Xe) are also likely to be atmospheric, but a final conclusion must wait until better data are obtained.In a 136Xe/130Xe−129Xe/130Xe diagram, diamond data lie on the same line as defined for MORB. The observed identical correlation for both diamonds and MORB's appears to suggest that the progenitor of the excess131–136Xe is 244Pu, but not238U, though the direct Xe isotopic measurements was not precies enough to decide unanimously the progenitor.  相似文献   

12.
Emissions from medical isotope production are the most important source of background for atmospheric radioxenon measurements, which are an essential part of nuclear explosion monitoring. This article presents a new approach for estimating the global annual radioxenon emission inventory caused by medical isotope production using the amount of Tc-99m applications in hospitals as the basis. Tc-99m is the most commonly used isotope in radiology and dominates the medical isotope production. This paper presents the first estimate of the global production of Tc-99m. Depending on the production and transport scenario, global xenon emissions of 11–45 PBq/year can be derived from the global isotope demand. The lower end of this estimate is in good agreement with other estimations which are making use of reported releases and realistic process simulations. This proves the validity of the complementary assessment method proposed in this paper. It may be of relevance for future emission scenarios and for estimating the contribution to the global source term from countries and operators that do not make sufficient radioxenon release information available. It depends on sound data on medical treatments with radio-pharmaceuticals and on technical information on the production process of the supplier. This might help in understanding the apparent underestimation of the global emission inventory that has been found by atmospheric transport modelling.  相似文献   

13.
Monitoring of radioactive noble gases, in particular xenon isotopes, is a crucial element of the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The capability of the noble gas network, which is currently under construction, to detect signals from a nuclear explosion critically depends on the background created by other sources. Therefore, the global distribution of these isotopes based on emissions and transport patterns needs to be understood. A significant xenon background exists in the reactor regions of North America, Europe and Asia. An emission inventory of the four relevant xenon isotopes has recently been created, which specifies source terms for each power plant. As the major emitters of xenon isotopes worldwide, a few medical radioisotope production facilities have been recently identified, in particular the facilities in Chalk River (Canada), Fleurus (Belgium), Pelindaba (South Africa) and Petten (Netherlands). Emissions from these sites are expected to exceed those of the other sources by orders of magnitude. In this study, emphasis is put on 133Xe, which is the most prevalent xenon isotope. First, based on the emissions known, the resulting 133Xe concentration levels at all noble gas stations of the final CTBT verification network were calculated and found to be consistent with observations. Second, it turned out that emissions from the radioisotope facilities can explain a number of observed peaks, meaning that atmospheric transport modelling is an important tool for the categorization of measurements. Third, it became evident that Nuclear Power Plant emissions are more difficult to treat in the models, since their temporal variation is high and not generally reported. Fourth, there are indications that the assumed annual emissions may be underestimated by factors of two to ten, while the general emission patterns seem to be well understood. Finally, it became evident that 133Xe sources mainly influence the sensitivity of the monitoring system in the mid-latitudes, where the network coverage is particularly good.  相似文献   

14.
Part I of this publication deals with the analysis of fission product releases consecutive to the Fukushima Dai-ichi accident. Reactor core damages are assessed relying on radionuclide detections performed by the CTBTO radionuclide network, especially at the particulate station located at Takasaki, 210 km away from the nuclear power plant. On the basis of a comparison between the reactor core inventory at the time of reactor shutdowns and the fission product activities measured in air at Takasaki, especially 95Nb and 103Ru, it was possible to show that the reactor cores were exposed to high temperature for a prolonged time. This diagnosis was confirmed by the presence of 113Sn in air at Takasaki. The 133Xe assessed release at the time of reactor shutdown (8 × 1018 Bq) turned out to be in the order of 80 % of the amount deduced from the reactor core inventories. This strongly suggests a broad meltdown of reactor cores.  相似文献   

15.
Preventing radioactive pollution is a troublesome problem but an urgent concern worldwide because radioactive substances cause serious health‐related hazards to human being. The adsorption method has been used for many years to concentrate and remove radioactive pollutants; selecting an adequate adsorbent is the key to the success of an adsorption‐based pollution abatement system. In Taiwan, all nuclear power plants use activated carbon as the adsorbent to treat radiation‐contaminated air emission. The activated carbon is entirely imported; its price and manufacturing technology are entirely controlled by international companies. Taiwan is rich in bamboo, which is one of the raw materials for high‐quality activated carbon. Thus, a less costly activated carbon with the same or even better adsorptive capability as the imported adsorbent can be made from bamboo. The objective of this research is to confirm the adsorptive characteristics and efficiency of the activated carbon made of Taiwan native bamboo for removing 131I gas from air in the laboratory. The study was conducted using new activated carbon module assembled for treating 131I‐contaminated air. The laboratory results reveal that the 131I removal efficiency for a single‐pass module is as high as 70%, and the overall efficiency is 100% for four single‐pass modules operated in series. The bamboo charcoal and bamboo activated carbon have suitable functional groups for adsorbing 131I and they have greater adsorption capacities than commercial activated carbons. Main mechanism is for trapping of radioiodine on impregnated charcoal, as a result of surface oxidation. When volatile radioiodine is trapped by potassium iodide‐impregnated bamboo charcoal, the iodo‐compound is first adsorbed on the charcoal surface, and then migrates to iodide ion sites where isotope exchange occurs.  相似文献   

16.
The abundance and isotopic composition of noble gases were determined in samples of CO2 well gas from Harding County, New Mexico. Our results confirm the presence of radiogenic129Xe and fissiogenic131–136Xe. Relative to noble gases in air, the CO2 gas is selectively depleted in the lighter weight, nonradiogenic noble gases, except at neon. It is suggested that loss of atmospheric neon into space could account for an apparent excess of neon in juvenile gases.  相似文献   

17.
Noble gas isotopes including 3He/4He, 40Ar/36Ar and Xe isotope ratios were determined for coexisting glass and olivine crystals in tholeiitic and alkalic basalts and dunite xenoliths from Loihi Seamount.Glass and coexisting olivine crystals have similar 3He/4He ratios (2.8–3.4) × 10?5, 20 to 24 times the atmospheric ratio (RA), but different 40Ar/36Ar ratios (400–1000). Based on the results of noble gas isotope ratios and microscopic observation, some olivine crystals are xenocrysts. We conclude that He is equilibrated between glass and olivine xenocrysts, but Ar is not.The apparent high 3He/4He ratio (3 × 10?5; = 21 RA) coupled with a relatively high 40Ar/36Ar ratio (4200) for dunite xenoliths (KK 17-5) may be explained by equilibration of He between MORB-type cumulates and the host magma.Except for the dunite xenoliths, noble gas data for these Loihi samples are compatible with a model in which samples from hot spot areas may be explained by mixing between P (plume)-type and M (MORB)-type components with the addition of A (atmosphere)-type component.Excess 129Xe has not been observed due to apparent large mass fractionation among Xe isotopes.  相似文献   

18.
Radon can be used as a naturally occurring tracer for environmental processes. By means of grab-sampling or continuous monitoring of radon concentration, it is possible to assess several types of dynamic phenomena in air and water. We present a review of the use of radon and its progeny at the University of Cantabria. Radon can be an atmospheric dynamics indicator related with air mass interchange near land-sea discontinuities as well as for the study of vertical variations of air parameters (average values of different types of stability: 131–580 Bq m?3). Concerning indoor gas, we present some results obtained at Altamira Cave (Spain): from 222 to 6549 Bq m?3 (Hall) and from 999 to 6697 Bq m?3 (Paintings Room). Finally, variations of radon concentration in soil (0.3 to 9.1 kBq m?3) and underground water (values up to 500 Bq l?1) provide relevant information about different geophysical phenomena.  相似文献   

19.
1.7 × 107yr-lived 129I has been positively detected in two natural tellurium ores by activation analysis with the help of low-level sum-coincidence gamma-ray spectrometry. The observed 129I concentrations can be explained as induced by muon reactions on 130Te. The detection of 129I provides for the first time conclusive evidence for the occurrence of natural long-lived muon-induced nuclides. Most of the 129Xe and 131Xe anomalies observed in natural tellurides are best interpreted in terms of reactions induced by muons and their secondary neutrons.  相似文献   

20.
Kr and Xe were measured by a stepwise heating technique in three samples of a drill core in the “Minnesota” fragment of the Estherville mesosiderite. The cosmogenic78Kr/83Kr decreased from the “top” sample to the “bottom” sample(“top” = 0.163 ± 0.005, “bottom” = 0.151 ± 0.005) while the cosmogenic131Xe/126Xe ratio increased(“top” = 5.58 ± 0.35, “bottom” = 6.92 ± 0.17). Cosmic-ray track studies have shown that the “top” sample was indeed closer to the preatmospheric surface than the “bottom” sample by ～ 10 cm. This is the first direct evidence, in a sample of known geometry, that the cosmogenic131Xe/126Xe ratio increases as a function of depth, and as such, confirms the hypothesis that the lunar131Xe anomaly is a bona fide depth effect due to resonance neutron capture in130Ba.  相似文献   

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