Global radioxenon emission inventory based on nuclear power reactor reports

Atmospheric radioactivity is monitored for the verification of the Comprehensive Nuclear-Test-Ban Treaty, with xenon isotopes ^131mXe, ¹³³Xe, ^133mXe and ¹³⁵Xe serving as important indicators of nuclear explosions. The treaty-relevant interpretation of atmospheric concentrations of radioxenon is enhanced by quantifying radioxenon emissions released from civilian facilities. This paper presents the first global radioxenon emission inventory for nuclear power plants, based on North American and European emission reports for the years 1995–2005. Estimations were made for all power plant sites for which emission data were unavailable. According to this inventory, a total of 1.3 PBq of radioxenon isotopes are released by nuclear power plants as continuous or pulsed emissions in a generic year.     

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.     

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.     

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.     

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.     

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.     

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.     

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.     

The influence of radiopharmaceutical isotope production on the global radioxenon background

Radioxenon isotopes play a major role in confirming whether or not an underground explosion was nuclear in nature. It is then of key importance to understand the sources of environmental radioxenon to be able to distinguish them from those of a nuclear explosion.     

Atmospheric xenon radioactive isotope monitoring

The Comprehensive Nuclear Test Ban Treaty (CTBT) organisation is implementing a world-wide monitoring network in order to check that the State Signatories comply with the treaty. One of the monitoring facilities consists of an atmospheric noble gas monitoring equipment. According to the requirements annexed in the treaty, the French Atomic Energy Commission (CEA) developed a device, called SPALAX, which automatically extracts xenon from ambient air and makes in situ measurements of the activities of four xenon radioisotopes (131mXe, 133mXe, 133Xe, 135Xe). The originality of this device is noticeable essentially in the gas sample processing method: thanks to the coupling of a gas permeator and of a noble gas specific adsorbent, it can selectively extract and concentrate xenon to more than 3 x 10 E6. This process is carried out continuously without cryogenic cooling, without any regeneration time. The detection of the xenon radioactive isotopes is done automatically by high spectral resolution gamma spectrometry, a robust technology well-suited for on-field instrumentation. In the year 2000, a prototype was involved in an international evaluation exercise directed by the CTBT organisation (CTBTO). This exercise demonstrated that the SPALAX equipment perfectly met the requirements of the CTBTO for such systems. On the basis of the continuous 24-h resolution record of the atmospheric xenon radioactive isotopes concentrations, the SPALAX system also demonstrated that ambient levels of 133Xe can fluctuate quickly from less than the detection limit to over 40 x 10(-3) Bq m(-3). In order to build an industrial version of this equipment, the CEA entered into a partnership with a French engineering company (S.F.I., Marseille, France), which is now able to produce an industrial version of SPALAX, i.e. more compact and more efficient than the prototypes. The 133Xe minimum detectable concentration is 0.15 x 10(-3) Bq m(-3) air per 24 h sampling cycle.     

Soil radium, soil gas radon and indoor radon empirical relationships to assist in post-closure impact assessment related to near-surface radioactive waste disposal

Least squares (LS), Theil’s (TS) and weighted total least squares (WTLS) regression analysis methods are used to develop empirical relationships between radium in the ground, radon in soil and radon in dwellings to assist in the post-closure assessment of indoor radon related to near-surface radioactive waste disposal at the Low Level Waste Repository in England. The data sets used are (i) estimated ²²⁶Ra in the <2 mm fraction of topsoils (eRa226) derived from equivalent uranium (eU) from airborne gamma spectrometry data, (ii) eRa226 derived from measurements of uranium in soil geochemical samples, (iii) soil gas radon and (iv) indoor radon data. For models comparing indoor radon and (i) eRa226 derived from airborne eU data and (ii) soil gas radon data, some of the geological groupings have significant slopes. For these groupings there is reasonable agreement in slope and intercept between the three regression analysis methods (LS, TS and WTLS). Relationships between radon in dwellings and radium in the ground or radon in soil differ depending on the characteristics of the underlying geological units, with more permeable units having steeper slopes and higher indoor radon concentrations for a given radium or soil gas radon concentration in the ground. The regression models comparing indoor radon with soil gas radon have intercepts close to 5 Bq m⁻³ whilst the intercepts for those comparing indoor radon with eRa226 from airborne eU vary from about 20 Bq m⁻³ for a moderately permeable geological unit to about 40 Bq m⁻³ for highly permeable limestone, implying unrealistically high contributions to indoor radon from sources other than the ground. An intercept value of 5 Bq m⁻³ is assumed as an appropriate mean value for the UK for sources of indoor radon other than radon from the ground, based on examination of UK data. Comparison with published data used to derive an average indoor radon: soil ²²⁶Ra ratio shows that whereas the published data are generally clustered with no obvious correlation, the data from this study have substantially different relationships depending largely on the permeability of the underlying geology. Models for the relatively impermeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with lower indoor radon: soil ²²⁶Ra ratios, whilst the models for the permeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with higher than average indoor radon: soil ²²⁶Ra ratios.     

Evaluation of selected monitoring methods for formaldehyde in domestic environments

Varioys analytical methodologies for the monitoring of formaldehyde (CH₂O) concentrations in domestic environments have been developed and evaluated. A modified CEA Instruments, Inc., analyzer has near-real-time CH₃O-specific analysis capability with an 0.01 mg/m³ detection limit. A solid sorbent, 13X molecular sieve has been utilized in a pumped collection unit with a demonstrated 0.03–12.5 mg/m³ linear dynamic range using sampling periods of ≤ 15 min. The development of screening-type techniques has included (1) a semipermeable-membrane passive sampler for measurements of average CH₂O concentrations over 8–24-h periods, and (2) a visual colorimetric analysis method for semiquantitative CH₂O determinations using solid chemical reagents. A preliminary field evaluation has been completed. The results show excellent agreement between the new CH₂O monitoring methods and a reference sampling and analysis technique. A generation apparatus for the production of CH₂O vapor is also reported with a demonstrated linear dynamic range between 0.003 and 12.5 mg/m³.     

The water footprint of sweeteners and bio-ethanol

An increasing demand for food together with a growing demand for energy crops result in an increasing demand for and competition over water. Sugar cane, sugar beet and maize are not only essential food crops, but also important feedstock for bio-ethanol. Crop growth requires water, a scarce resource. This study aims to assess the green, blue and grey water footprint (WF) of sweeteners and bio-ethanol from sugar cane, sugar beet and maize in the main producing countries. The WFs of sweeteners and bio-ethanol are mainly determined by the crop type that is used as a source and by agricultural practise and agro-climatic conditions; process water footprints are relatively small. The weighted global average WF of sugar cane is 209 m³/tonne; for sugar beet this is 133 m³/tonne and for maize 1222 m³/tonne. Large regional differences in WFs indicate that WFs of crops for sweeteners and bio-ethanol can be improved. It is more favourable to use maize as a feedstock for sweeteners or bio-ethanol than sugar beet or sugar cane. The WF of sugar cane contributes to water stress in the Indus and Ganges basins. In the Ukraine, the large grey WF of sugar beet contributes to water pollution. In some western European countries, blue WFs of sugar beet and maize need a large amount of available blue water for agriculture. The allocation of the limited global water resources to bio-energy on a large scale will be at the cost of water allocation to food and nature.     

Weather-dependent change of cesium,strontium, barium and tellurium contamination deposited as aerosols on various cultures

Various types of plants (wheat, bean, lettuce, radish and grass) were contaminated by dry deposition of radioactive aerosols (¹³⁷Cs, ⁸⁵Sr, ¹³³Ba and ^123mTe) in order to supplement the radioecological data necessary for operational post-accidental codes. A few days after deposition, rainfalls were applied to these cultures to evaluate the influence of some characteristics of the rain on the contamination of the culture over time. On the other hand, for wheat and bean, the influence of the humidity condition of the foliage at the contamination time was considered. For a given plant species at a given vegetative stage, the four radionuclides were intercepted in an identical way. The interception varied from 30% for bean (young sprout) to 80% for lettuce (near maturity). The global transfer factor values were dependent on both the radionuclides and the plant species; nevertheless, a higher value was obtained for cesium, regardless of the plant and the rainfall (from 0.006 m² kg_fresh⁻¹ for wheat-grains – contaminated at the shooting stage – or for bean-pods – contaminated at the pre-flowering stage – to 0.1 m² kg_fresh⁻¹ for a whole lettuce). The analysis of the results allowed us on the one hand, to extract parameter values of the foliar transfer directly usable in operational codes, in particular those relating to barium and tellurium, unknown until then, and on the other hand, to lay the foundations of a future, more mechanistic model, taking into account the foliar processes in a finer way.     

Cocaine and cannabinoids in the atmosphere of Northern Europe cities,comparison with Southern Europe and wastewater analysis

This study reports the first investigation of atmospheric illicit drug concentrations in Northern Europe using measurements of cocaine and cannabinoids in Amsterdam, London and Stockholm. Further, these measurements were compared to those made in Rome to explore the geographical and inter-city variability. Co-located measurements of atmospheric particulate mass and PAHs were used to help describe and interpret the illicit drug measurements with respect to atmospheric dispersion. Cocaine concentrations ranged from 0.03 to 0.14 ng/m³ in Amsterdam, from 0.02 to 0.33 ng/m³ in London and were below quantification limit (3 pg/m³) in Stockholm. Cannabinol was the only cannabinoid molecule detected in the three cities. During this campaign, London reported the highest concentrations of cocaine and meaningful differences were detected between the urban background and city centre London sites. Mean cocaine concentrations measured in Amsterdam during March 2011 were also compared with those measured simultaneously in eight Italian cities. The cocaine concentration in Amsterdam was comparable to that measured at an urban background in Milan and at a densely populated site in Florence. Although correlating atmospheric concentrations directly with drug prevalence is not possible using current data, links between concentrations of cocaine and estimates of abuse prevalence assessed by the more routinely used wastewater analysis were also examined. A statistically significant correlation was found between the two sets of data (R² = 0.66; p = 0.00131). Results confirmed that meteorology, population rate and habits of consumption influence the atmospheric concentrations of drugs. If these confounding factors were better controlled for, the techniques described here could became an easy and cost effective tool to index the impact of cocaine abuse in the area; especially where local hot spots need to be identified.     

Contrasting cesium dynamics in neighboring deep and shallow warm-water reservoirs

To measure the long term retention and seasonal dynamics of an initial 4 kg addition of ¹³³Cs into an 11.4-ha, 157,000 m³ reservoir (Pond 4, near Aiken, South Carolina, USA), the concentrations and inventories of ¹³³Cs in the water column were measured at periodical intervals for 522 days following the 1 August, 1999 release. After rapid declines in concentrations and inventories during the first 90 days, the ¹³³Cs concentrations in the water column declined at an average proportional rate of 0.004 d⁻¹. However, there were periods of less rapid and more rapid rates of declines, and these were correlated with periods of increasing and decreasing K concentrations in the water column. The decline rates were less and the K concentrations greater in the winter than in the summer. In the deeper, neighboring monomictic reservoirs of Par Pond and Pond B, a yearly cycle of increasing and decreasing ¹³⁷Cs concentrations in the water column is driven by anoxic remobilization of Cs from the sediments into a persistent summer hypolimnion. In Pond 4, whose mean depth of 1.6 m is too shallow to support a persistent anoxic hypolimnion, the pattern of yearly dynamics for K and Cs appear to be related to the accumulation and release of these elements from the extensive, seasonal macrophyte communities. The contrasting results between Pond 4 and Pond B suggest that a full appreciation of the relative importance of 1) anoxic remobilization and 2) accumulation and release by macrophytes in these systems remains to be established.     

Considerations in deriving quantitative cancer criteria for inorganic arsenic exposure via inhalation

The inhalation unit risk (IUR) that currently exists in the United States Environmental Protection Agency's (US EPA's) Integrated Risk Information System was developed in 1984 based on studies examining the relationship between respiratory cancer and arsenic exposure in copper smelters from two US locations: the copper smelter in Anaconda, Montana, and the American Smelting And Refining COmpany (ASARCO) smelter in Tacoma, Washington. Since US EPA last conducted its assessment, additional data have become available from epidemiology and mechanistic studies. In addition, the California Air Resources Board, Texas Commission of Environmental Quality, and Dutch Expert Committee on Occupational Safety have all conducted new risk assessments. All three analyses, which calculated IURs based on respiratory/lung cancer mortality, generated IURs that are lower (i.e., less restrictive) than the current US EPA value of 4.3 × 10^− 3 (μg/m³)^− 1. The IURs developed by these agencies, which vary more than 20-fold, are based on somewhat different studies and use different methodologies to address uncertainties in the underlying datasets. Despite these differences, all were developed based on a cumulative exposure metric assuming a low-dose linear dose–response relationship. In this paper, we contrast and compare the analyses conducted by these agencies and critically evaluate strengths and limitations inherent in the data and methodologies used to develop quantitative risk estimates. In addition, we consider how these data could be best used to assess risk at much lower levels of arsenic in air, such as those experienced by the general public. Given that the mode of action for arsenic supports a threshold effect, and epidemiological evidence suggests that the arsenic concentration in air is a reliable predictor of lung/respiratory cancer risk, we developed a quantitative cancer risk analysis using a nonlinear threshold model. Applying a nonlinear model to occupational data, we established points of departure based on both cumulative exposure (μg/m³-years) to arsenic and arsenic concentration (μg/m³) via inhalation. Using these values, one can assess the lifetime risk of respiratory cancer mortality associated with ambient air concentrations of arsenic for the general US population.     

Radon exhalation from building materials for decorative use

Long-term exposure to radon increases the risk of developing lung cancer. There is considerable public concern about radon exhalation from building materials and the contribution to indoor radon levels. To address this concern, radon exhalation rates were determined for 53 different samples of drywall, tile and granite available on the Canadian market for interior home decoration. The radon exhalation rates ranged from non-detectable to 312 Bq m⁻² d⁻¹. Slate tiles and granite slabs had relatively higher radon exhalation rates than other decorative materials, such as ceramic or porcelain tiles. The average radon exhalation rates were 30 Bq m⁻² d⁻¹ for slate tiles and 42 Bq m⁻² d⁻¹ for granite slabs of various types and origins. Analysis showed that even if an entire floor was covered with a material having a radon exhalation rate of 300 Bq m⁻² d⁻¹, it would contribute only 18 Bq m⁻³ to a tightly sealed house with an air exchange rate of 0.3 per hour. Generally speaking, building materials used in home decoration make no significant contribution to indoor radon for a house with adequate air exchange.     

Aluminum, iron, and lead content of respirable particulate samples from a personal monitoring study

Samples of respirable particulate matter collected during a personal monitoring study in Topeka, KS, were analyzed for iron, aluminum, and lead content. The sampling protocol and instrumentation are described in detail. Lead indoor concentrations (median = 79 ng/m³) were found to be less than both personal (median = 112 ng/m³) and outdoor lead concentrations (median = 106 ng/m³). The indoor, outdoor, and personal levels of iron and aluminum were not significantly different. In addition, it was determined that outdoor respirable particulate mass does not correlate well with the personal or indoor metal concentrations, and that the amount of time spent in motor vehicles is a relatively good indicator of lead exposures. The relationships between indoor, outdoor, and personal lead are discussed in greater detail, with references to supporting evidence from other studies.