Xenon isotopic signature study of the primary coolant of CANDU nuclear power plant to enhance CTBT verification

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.     

Krypton isotopic signature study of the primary coolant of CANDU nuclear power plant

To support interpretation of observed atmospheric krypton radioisotopes, a database of krypton radioisotope in the primary coolant of CANDU reactors has been established. This database is comprised of 40,000 records of high-quality ⁸⁹Kr, ⁸⁷Kr, ⁸⁸Kr and ^85mKr 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 krypton radioisotopes in the CANDU reactor primary coolant. These studies provided practical information on the characterization of CANDU reactor krypton radioisotope, which can potentially be used to discriminate between reactor effluent and fuel reprocessing for nuclear safeguard ⁸⁵Kr monitoring applications (Kalinowski et al., J Environ Radioact 73:203, 2004). The study also has some potential application to Fissile material cut-off treaty.     

Determination of in-core power in low energy research reactors by measurement of16N and18F in the primary coolant

The measurement of¹⁶N and¹⁸F activity in the primary coolant of the JASON Argonaut reactor has been used to monitor in-core reactor power. The¹⁶N is produced by the¹⁶O(n, p)¹⁶N reaction and the 6.1 MeV photopeak was measured on-line using a BGO detector adjacent to the primary coolant circuit. These data provided a relative measure of power stability during steady state operation and a measure of linearity at different power levels. The¹⁸F is produced in the primary coolant by the¹⁸O(p, n)¹⁸F reaction and aliquots of primary coolant were sampled from the reactor dump tank for off-line radiochemical analysis. The¹⁸F was separated as trimethylfluorosilane and the activity was determined by measurement of the 0.511 MeV annihilation photopeak using a NaI(TI) detector. The measured¹⁸F activity was used to determine actual in-core reactor power using both ab-initio calculations and by comparison of results with a calibrated power reactor. The¹⁸F data also provided a method of nomalising the¹⁶N data for direct monitoring of in-core reactor power in JASON.     

Speciation and estimation of radioiodine in reactor coolant water

The species of radioiodine in the primary coolant water of the heavy water moderated, heavy water cooled 100 MW research reactor have been identified. It was observed that IO ₃ ^? was the major species in the reactor coolant during reactor operation and I^? was the major species during shutdown. Organic and elemental forms amount only to less than 2% of total radioiodine. A simple method was developed for the estimation of gross iodine activity in reactor coolant water. The method involves the separation of all inorganic forms of iodine into a photographic film consisting of a thin layer of silver halide. The iodine in the film was estimated by gross counting of the film in a Geiger-Müller counter. Gross iodine activity in the reactor coolant samples estimated by the present method were in agreement with that obtained by direct γ-spectrometry with a Ge detector. It is concluded that the method can be used for the routine estimation of radioiodine in reactor coolant water.¹³³I/¹³¹I and¹³⁵I/¹³¹I ratios in the film were estimated and found to be useful in identifying split rod conditions in the reactor.     

Estimating the four-factor product (ε p P<Subscript>fnl</Subscript> P<Subscript>tnl</Subscript>) for the accurate calculation of xenon and samarium reactivities in the Syrian Miniature Neutron Source Reactor

The modified ¹³⁵Xe equilibrium reactivity in the Syrian Miniature Neutron Source Reactor (MNSR) was calculated first by using the WIMSD4 and CITATION codes to estimate the four-factor product (ε p P _fnl P _tnl ). Then, precise calculations of ¹³⁵Xe and ¹⁴⁹Sm concentrations and reactivities were carried out and compared during the reactor operation time and after shutdown. It was found that the ¹³⁵Xe and ¹⁴⁹Sm reactivities did not reach their equilibrium reactivities during the daily operating time of the reactor. The ¹⁴⁹Sm reactivities could be neglected compared to ¹³⁵Xe reactivities during the reactor operating time and after shutdown.     

Research reactors as sources of atmospheric radioxenon

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.     

Xe-135 production from Cf-252

The presence of ¹³⁵Xe is often used as an indicator that fission has occurred, and is used to help enforce the Comprehensive Test Ban Treaty. There are no known commercial suppliers, though it can be acquired. Readily available standards of this isotope are very useful. ¹³⁵Xe can be produced through fission, or by neutron capture on ¹³⁴Xe. At the INL, scientists have previously transported fission products from an electroplated ²⁵²Cf thin source for the measurement of nuclear data of short-lived fission products using a technique called He-Jet collection. A similar system has been applied to the collection of gaseous ¹³⁵Xe, and ¹³³Xe, in order to produce standards of these isotopes.     

Beta-gamma counting system for Xe fission products

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 the^131mXe,^133gXe,^133mXe, and^135gXe 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.     

Radioxenon production through neutron irradiation of stable xenon gas

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.     

Contributions to the 37Ar background by research reactor operations

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.     

SDAT implementation for the analysis of radioxenon β–γ coincidence spectra

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.     

Application of BGO detector to monitor in situ16N concentration in a reactor pool

A high efficiency BGO detecting system coupled to a coolant pumping device was used to monitor on-line the 6.13 MeV high energy gamma-ray, which is emitted from the 7.1 s half-life of¹⁶N activated by¹⁶O(n, p) reaction in a nuclear reactor. The system has been demonstrated effectively to monitor the real-time reactor power level as well as the space-time neutron flux distribution in reactor coolant.     

Field testing of collection and measurement of radioxenon for the Comprehensive Test Ban Treaty

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.     

Plurality of radiation-chemical steady states during the radiolysis of water coolant in nuclear reactor

A computational study has been performed on the radiolysis of an aqueous solution that has the chemical composition and irradiation parameters typical of the primary coolant of pressurized water reactors. In this work, in contrast to previous studies on this subject, it has been taken into account that temporary fluctuations of the reactor radiation parameters, such as the composition of reactor n, γ]-radiation and the absorbed dose rate in the coolant, may occur in an actual real reactor during irradiation. The feasibility of spontaneous switching of the radiation-chemical system from one steady state with low concentrations of oxidizing products of radiolysis to another state with high concentrations resulting from a spike of the reactor radiation dose rate against the background of constant dose rate before and after the spike has been shown. The event triggering the switch is an increase in the concentration of oxygen and HO₂ (O₂^–) radicals during the spike, after which the positive feedback does not allow the system to return back to the initial steady state. In practice, this effect can be caused by phenomena associated with local irregularities in the reactor core: the composition and dose rate of reactor radiation, the presence of steam–gas bubbles due to local subcooled nucleate boiling of the coolant in the core, and the perturbation of the water radiolysis mechanism at the surface of fuel rods because of an increased contribution of heterogeneous reactions etc.     

Dating the age of a recent nuclear event by gamma-spectrometry

Summary The age of a recent, i.e., fresh, nuclear event can be determined by measuring the activity of short-lived parent and daughter fission products. The event studied was a short irradiation, of a small sample of uranium, in a nuclear reactor. Two clocks were investigated, ⁹²Sr-⁹²Y and ¹³⁵I-¹³⁵Xe. Measurements of the source by gamma-spectrometry yielded very good agreement between true and measured ages. The upper and lower age limits of applicability for the clocks in question were defined. The half-life of ⁹²Sr was found 2.635±0.008 hours and of ¹³⁵I 6.65±0.04 hours.     

Migration of fission product137Cs in mud near a nuclear reactor

Due to the mismanagement of nuclear waste as well as heat exchanger degradation for the primary coolant of the one megawatt nuclear research reactor, the fission product¹³⁷Cs has been leaking to the environment ever since 1969. In the past thirty years, the long-lived¹³⁷Cs was accumulated and eventually trapped in the mud of the discharge pond right in front of the waste storage and the reactor facility. The distribution of¹³⁷Cs in mud was measured and contour-mapped to reveal the migration of trace levels of¹³⁷Cs in a period of three decades.     

The pre-Fermi natural reactor: A note on the periodic mode of operation

The isotopic compositions of xenon released from the Oklo reactor at temperatures below 1000°C are such that the abundances of¹³¹Xe,¹³²Xe and¹³⁴Xe relative to¹³⁶Xe are markedly enhanced when compared to the relative fission yields from the thermal neutron-induced fission of²³⁵U. These anomalies can be attributed to the fact that¹³¹Xe,¹³²Xe and¹³⁴Xe have fairly long-lived precursors: 8.04-day¹³¹I, 78.2-hour¹³²Te and 42-minute¹³⁴Te, respectively. It is possible to determine the duration of the time when the reactor was turned off from the ratios of excess¹³²Xe to excess¹³⁴Xe in these anomalous xenon fractions released from the Oklo reactor. Calculations based on the available xenon isotope data that the time period during which the reactor was turned off was approximately 2 to 3 hours.     

The ENEA noble gas laboratory: status of implementation

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.     

Measurement of <Superscript>90</Superscript>Sr in primary coolant of pressurized water reactor

The present procedure for analysing ⁹⁰Sr combines the use of a non radioactive carrier with high pressure ion chromatography separation, conductivity detection of the carrier and optimized external counting by liquid scintillation. This improvement with respect to traditional methods led to a more rapid and efficient purification stage. The present work proves that activities of ⁹⁰Sr as low as 3 Bq/L can be measured in highly contaminated pressurized water reactor primary coolant matrix without any observed radiochemical interference. The approach shows promise for the analysis of other emitters of low energy radiation, or isotopes subject to high background or matrix effects in a PWR primary coolant.