The influence on the radioxenon background during the temporary suspension of operations of three major medical isotope production facilities in the Northern Hemisphere and during the start-up of another facility in the Southern Hemisphere

Medical isotope production facilities (MIPF) have recently been identified to emit the major part of the environmental radioxenon measured at many globally distributed monitoring sites deployed to strengthen the radionuclide component of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) verification regime. Efforts to raise a global radioxenon emission inventory revealed that the yearly global total emission from MIPF’s is around 15 times higher than the total radioxenon emission from nuclear power plants (NPP's).Given that situation, from mid 2008 until early 2009 two out of the ordinary hemisphere-specific events occured:1) In the Northern hemisphere, a joint temporary suspension of operations of the three largest MIPF's made it possible to quantify the effects of the emissions related to NPP’s. The average activity concentrations of ¹³³Xe measured at a monitoring station close to Freiburg, Germany, went down significantly from 4.5 ± 0.5 mBq/m³ to 1.1 ± 0.1 mBq/m³ and in Stockholm, Sweden, from 2.0 ± 0.4 mBq/m³ to 1.05 ± 0.15 mBq/m³.2) In the Southern hemisphere the only radioxenon-emitting MIPF in Australia started up test production in late November 2008. During eight test runs, up to 6.2 ± 0.2 mBq/m³ of ¹³³Xe was measured at the station in Melbourne, 700 km south-west from the facility, where no radioxenon had been observed before, originating from the isotopic production process.This paper clearly confirms the hypothesis that medical isotope production facility are at present the major emitters of radioxenon to the atmosphere. Suspension of operations of these facilities indicates the scale of their normal contribution to the European radioxenon background, which decreased two to four fold. This also gives a unique opportunity to detect and investigate the influence of other local and long distance sources on the radioxenon background. Finally the opposing effect was studied: the contribution of the start-up of a renewed radiopharmaceutical facility to the build up of a radioxenon background across Australia and the Southern hemisphere.     

Machine learning for radioxenon event classification for the Comprehensive Nuclear-Test-Ban Treaty

A method of weapon detection for the Comprehensive nuclear-Test-Ban-Treaty (CTBT) consists of monitoring the amount of radioxenon in the atmosphere by measuring and sampling the activity concentration of ^131mXe, ¹³³Xe, ^133mXe, and ¹³⁵Xe by radionuclide monitoring. Several explosion samples were simulated based on real data since the measured data of this type is quite rare. These data sets consisted of different circumstances of a nuclear explosion, and are used as training data sets to establish an effective classification model employing state-of-the-art technologies in machine learning. A study was conducted involving classic induction algorithms in machine learning including Naïve Bayes, Neural Networks, Decision Trees, k-Nearest Neighbors, and Support Vector Machines, that revealed that they can successfully be used in this practical application. In particular, our studies show that many induction algorithms in machine learning outperform a simple linear discriminator when a signal is found in a high radioxenon background environment.     

Evaluation of radioxenon releases in Australia using atmospheric dispersion modelling tools

The origin of a series of atmospheric radioxenon events detected at the Comprehensive Test Ban Treaty Organisation (CTBTO) International Monitoring System site in Melbourne, Australia, between November 2008 and February 2009 was investigated. Backward tracking analyses indicated that the events were consistent with releases associated with hot commission testing of the Australian Nuclear Science Technology Organisation (ANSTO) radiopharmaceutical production facility in Sydney, Australia. Forward dispersion analyses were used to estimate release magnitudes and transport times. The estimated ¹³³Xe release magnitude of the largest event (between 0.2 and 34 TBq over a 2 d window), was in close agreement with the stack emission releases estimated by the facility for this time period (between 0.5 and 2 TBq). Modelling of irradiation conditions and theoretical radioxenon emission rates were undertaken and provided further evidence that the Melbourne detections originated from this radiopharmaceutical production facility. These findings do not have public health implications. This is the first comprehensive study of atmospheric radioxenon measurements and releases in Australia.     

Aerial measurement of radioxenon concentration off the west coast of Vancouver Island following the Fukushima reactor accident

In response to the Fukushima nuclear reactor accident, on March 20th, 2011, Natural Resources Canada conducted aerial radiation surveys over water just off the west coast of Vancouver Island. Dose-rate levels were found to be consistent with background radiation, however a clear signal due to ¹³³Xe was observed. Methods to extract ¹³³Xe count rates from the measured spectra, and to determine the corresponding ¹³³Xe activity concentration, were developed. The measurements indicate that ¹³³Xe concentrations on average lie in the range of 30-70 Bq/m³.     

Isotopic signature of atmospheric xenon released from light water reactors

A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System to verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The isotopic activity ratios of (135)Xe, (133m)Xe, (133)Xe and (131m)Xe are of interest for distinguishing nuclear explosion sources from civilian releases. Simulations of light water reactor (LWR) fuel burn-up through three operational reactor power cycles are conducted to explore the possible xenon isotopic signature of nuclear reactor releases under different operational conditions. It is studied how ratio changes are related to various parameters including the neutron flux, uranium enrichment and fuel burn-up. Further, the impact of diffusion and mixing on the isotopic activity ratio variability are explored. The simulations are validated with reported reactor emissions. In addition, activity ratios are calculated for xenon isotopes released from nuclear explosions and these are compared to the reactor ratios in order to determine whether the discrimination of explosion releases from reactor effluents is possible based on isotopic activity ratios.     

Automated radioxenon monitoring for the comprehensive nuclear-test-ban treaty in two distinctive locations: Ottawa and Tahiti

In preparation for verification of the Comprehensive Nuclear-Test-Ban-Treaty, automated radioxenon monitoring is performed in two distinctive environments: Ottawa and Tahiti. These sites are monitored with SPALAX (Systeme de Prelevement d'air Automatique en Ligne avec l'Analyse des radioXenons) technology, which automatically extracts radioxenon from the atmosphere and measures the activity concentrations of (131m,133m,133,135)Xe. The resulting isotopic concentrations can be useful to discern nuclear explosions from nuclear industry xenon emissions. Ambient radon background, which may adversely impact analyser sensitivity, is discussed. Upper concentration limits are reported for the apparently radioxenon free Tahiti environment. Ottawa has a complex radioxenon background due to proximity to nuclear reactors and medical isotope facilities. Meteorological models suggest that, depending on the wind direction, the radioxenon detected in Ottawa can be characteristic of the normal radioxenon background in the Eastern United States, Europe, and Japan or distinctive due to medical isotope production.     

Elevated radioxenon detected remotely following the Fukushima nuclear accident

We report on the first measurements of short-lived gaseous fission products detected outside of Japan following the Fukushima nuclear releases, which occurred after a 9.0 magnitude earthquake and tsunami on March 11, 2011. The measurements were conducted at the Pacific Northwest National Laboratory (PNNL), (46°16′47″N, 119°16′53″W) located more than 7000 km from the emission point in Fukushima Japan (37°25′17″N, 141°1′57″E). First detections of ¹³³Xe were made starting early March 16, only four days following the earthquake. Maximum concentrations of ¹³³Xe were in excess of 40 Bq/m³, which is more than ×40,000 the average concentration of this isotope is this part of the United States.     

Detection and analysis of xenon isotopes for the comprehensive nuclear-test-ban treaty international monitoring system

The use of the xenon isotopes for detection of nuclear explosions is of great interest for monitoring compliance with the comprehensive nuclear-test-ban treaty (CTBT). Recently, the automated radioxenon sampler-analyzer (ARSA) was tested at the Institute for Atmospheric Radioactivity (IAR) in Freiburg, Germany to ascertain its use for the CTBT by comparing its results to laboratory-based analyses, determining its detection sensitivity and analyzing its results in light of historical xenon isotope levels and known reactor operations in the area. Xe-133 was detected nearly every day throughout the test at activity concentrations ranging between approximately 0.1 mBq/m3 to as high as 120 mBq/m3. Xe-133m and 135Xe were also detected occasionally during the test at concentrations of less than 1 to a few mBq/m3.     

Occurrence and behaviour of radionuclides in the Moselle River—Part III: Dispersion of radionuclides along the river course

Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with ⁵⁸Co, ⁶⁰Co and ^110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.     

Sources of anthropogenic radionuclides in the environment: a review

Studies of radionuclides in the environment have entered a new era with the renaissance of nuclear energy and associated fuel reprocessing, geological disposal of high-level nuclear wastes, and concerns about national security with respect to nuclear non-proliferation. This work presents an overview on sources of anthropogenic radionuclides in the environment, as well as a brief discussion of salient geochemical behavior of important radionuclides. We first discuss the following major anthropogenic sources and current developments that have lead, or could potentially contribute, to the radionuclide contamination of the environment: (1) nuclear weapons program; (2) nuclear weapons testing; (3) nuclear power plants; (4) uranium mining and milling; (5) commercial fuel reprocessing; (6) geological repository of high-level nuclear wastes that include radionuclides might be released in the future, and (7) nuclear accidents. Then, we briefly summarize the inventory of radionuclides ⁹⁹Tc and ¹²⁹I, as well as geochemical behavior for radionuclides ⁹⁹Tc, ¹²⁹I, and ²³⁷Np, because of their complex geochemical behavior, long half-lives, and presumably high mobility in the environment; biogeochemical cycling and environment risk assessment must take into account speciation of these redox-sensitive radionuclides.     

Overview of strontium-89,90 deposition measurements in Finland 1963-2005

In Finland the deposition of strontium-89 (⁹⁰Sr) and strontium-90 (⁹⁰Sr) has been monitored since the early 1960s. The measured cumulative ⁹⁰Sr deposition in 1963-2005 is on average 1200 Bq m⁻², of which 150 Bq m⁻² originates from the Chernobyl accident. Adding to this the deposition in 1945-1962 produces a value of 2040 Bq m⁻² for the cumulative deposition in Finland. The nuclear explosion-derived deposition up to 1985 obtained in this study, 1850 Bq m⁻², is in good agreement with the zonal ⁹⁰Sr deposition of 1740 Bq m⁻² in the 60°N-70°N latitude band estimated by UNSCEAR. The regional deposition patterns of ⁸⁹Sr and ⁹⁰Sr following the Chernobyl accident resemble those of the refractory nuclides such as ^239,240Pu and ⁹⁵Zr. The total deposition of Chernobyl-derived ⁹⁰Sr in Finland was about 5.3 × 10¹³ Bq. This activity corresponds to 0.027% of the reactor core inventory and 0.66% of the atmospheric emissions from the accident. The corresponding figures for ⁸⁹Sr are 4.5 × 10¹⁴ Bq, 0.023% and 0.56%, respectively.     

C, δC and total C content in soils around a Brazilian PWR nuclear power plant

Nuclear power plants release ¹⁴C during routine operation mainly as airborne gaseous effluents. Because of the long half-life (5730 years) and biological importance of this radionuclide (it is incorporated in plant tissue by photosynthesis), several countries have monitoring programs in order to quantify and control these emissions. This paper compares the activity of ¹⁴C in soils taken within 1 km from a Brazilian nuclear power plant with soils taken within a reference area located 50 km away from the reactor site. Analyses of total carbon, δ¹³C and ¹³⁷Cs were also performed in order to understand the local soil dynamics. Except for one of the profiles, the isotopic composition of soil organic carbon reflected the actual forest vegetation present in both areas. The ¹³⁷Cs data show that the soils from the base of hills are probably allocthonous.     

Atmospheric releases from fossil fuel power plants in the United States

This paper contains detailed data on atmospheric emissions from power plants with a capacity of more than 25 MW electric in the United States. The data are gathered from utility files as presented to the U.S. Environmental Protection Agency. Pollutants covered are CO, NO_x, SO_x3, particulates, and total hydrocarbons. The data indicate that in 1977 about 420×10⁹ kg coal, 84×10⁶ m³ oil, and 65×10⁶ m³ of natural gas were used to generate electricity. Pollutants generated were 2×10⁹kg particulates, 17×10⁹ kg SO₂, 6×10⁹ kg NO_x, 78×10⁶ kg hydrocarbons and 0.3×10⁶ kg of CO.     

Fission Product tin in sediments

We describe a method for the determination of long-lived tin isotopes arising from nuclear fission. The isotopes are extracted from sediments with hydrochloric acid and separated by methylisobutylketone extraction, ion-exchange chromatography, precipitation of cesium hexachlorostannate and ferric hydroxide coprecipitation. The 100 000-year ¹²⁶Sn was not detected but beta activity consistent with ^121mSn (55 year) was found in sediment samples from a location known to be contaminated with fission products.     

Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China

The total ^239+240Pu activities and ²⁴⁰Pu/²³⁹Pu atom ratios in surface soil samples (0–5 cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, ^239+240Pu activities in fine particles (<150 μm) were 1.3–2.1 times of those in coarse particles (150 μm–1 mm) which ranged from 0.005 to 0.157 mBq/g. Atom ratios of ²⁴⁰Pu/²³⁹Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182 ± 0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean ²⁴⁰Pu/²³⁹Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, ^239+240Pu activities in the various layers ranged from 0.012 to 0.23 mBq/g, and the inventory of ^239+240Pu (32.4 Bq/m², 0–23 cm) was slightly lower than that expected from global fallout (42 Bq/m²) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10–23 cm) was as high as 83%. The ^239+240Pu activity levels and ²⁴⁰Pu/²³⁹Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas

Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of ^239+240Pu and the atom ratios of ²⁴⁰Pu/²³⁹Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ²⁴⁰Pu/²³⁹Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of ^239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m²) and the Sulu Sea (1.38 Bq/m²). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.     

Estimation of the nutrient inputs into river systems – experiences from German rivers

The nutrient discharges from point and diffuse sources in more than 200 German river basins were estimated for the periods 1983–1987 and 1993–1997 employing the MONERIS model. This model distinguishes between six diffuse pathways and point source emissions from waste water treatment plants and direct industrial discharges. It was estimated that the total nitrogen input into the German river systems amounts to about 819,000 t N year^–1 in the period 1993 to 1997. These emissions have decreased since the mid-eighties by about 266,000 t N year^–1, mainly caused by the reduction of point discharges. For phosphorus the emissions have been reduced by 56,290 t P year^–1 and amount to 37,250 t P year^–1 in the period 1993–1997. Based on emission data a retention module estimates riverine nutrient loads. The comparison of the model output with the observed loads shows a deviation as low as 30% and 50% for nitrogen and phosphorus, respectively. The regional resolution of the model indicates the relative importance of different pathways for phosphorus and nitrogen input into river systems. Electronic Publication     

CO2 dispersion around two PWR nuclear power plants in Brazil

Atmospheric air samples were taken within 3 km from power plants encompassing five different distances and wind directions. Samples were taken between 2002 and 2005 aiming to evaluate the environmental ¹⁴C enrichment due to the operation of Brazilian nuclear power plants. The sampling system consisted of a pump connected to a trapping column filled with a 3 M NaOH solution. The trapped CO₂ was analyzed for ¹⁴C by using a single stage accelerator mass spectrometry (SSAMS).     

Energy analysis for onsite and offsite suburban wastewater

The environmental consequence of meeting the planet’s energy requirements has shown that biological degradation of organic constituent from wastewater does not only produces biogas. It also produces flammable methane that has 21 times more global warming potential or greenhouse effect than carbon dioxide. This becomes a loss of potential renewable energy when it is flared. This study investigates recoverable energy from cassava wastewater and effect of unrecovered onsite (not from treatment plant) wastewater energy. Sludge from both onsite untreated and offsite treated wastewater from a cassava processing station in a sub urban community of Nigeria was analyzed. The result shows that the offsite treatment has a methane potential of 27.428 m³/day compared to the onsite methane emission potential with 17.807 m³/day. The onsite 17.807 m³/day of methane is equivalent to 0.126 kgCH₄/year of emitted methane base on industrial procedure standards by the IPCC (2006) guidelines for national greenhouse gas inventories. An additional 54.03% of methane will be recovered if the onsite emissions were to be captured . At an emission efficiency of 0.025 kgCH₄/kg COD, the untreated wastewater indicates a potential contribution to the greenhouse effect. A mathematical model analysis was presented for ease in determining the amount of methane emitted from the untreated wastewater. This study support suggested methodologies and previous work comparing anaerobic offsite methane potential and untreated wastewater methane emission potentials along with its greenhouse effects.