Krypton-85 in the atmosphere 1950–1977: a data review

For over 20 years the radioactive noble gas ⁸⁵Kr, the product of nuclear industry, has been released to the environment mainly from nuclear fuel reprocessing plants. Owing to its relatively long half-life $\text{T(}\text{1}\text{2}\text{= 10.76}\text{y}\text{)}$ and the absence of other appreciable sinks, a cumulative buildup of ⁸⁵Kr in the atmosphere is observed. The mean ⁸⁵Kr surface air activity in the northern hemisphere has increased from about 20 dpm/mmol Kr in 1950 to about 750 dpm/mmol Kr in 1977. In recent years, a substantial slow-down of the ⁸⁵Kr emission rate to the atmosphere has been observed. The published data indicate rather good mixing of ⁸⁵Kr in the northern hemisphere, but a gradient is observed in the southern hemisphere due to the fact that all nuclear fuel reprocessing plants are situated in the northern hemisphere and due to poor mixing of the atmosphere in the meridional direction.This paper summarizes nearly all of the data on ⁸⁵Kr activity in the atmosphere published up to the middle of 1978. The spatio-temporal distribution of ⁸⁵Kr atmospheric activity is discussed. Some forecasts of future ⁸⁵Kr concentration in the atmosphere and its possible ecological consequences are also presented.     

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.     

In situ metrology of 85Kr plumes released by the COGEMA La Hague nuclear reprocessing plant

The IRSN (Institut de Radioprotection et de S?reté Nucléaire, France) has started an in situ study of the behaviour of atmospheric releases close-by the COGEMA La Hague nuclear reprocessing plant. The study is designed to improve information on the dispersion of radioactive pollutants very close to the emission point--a 100 m height chimney. In this situation, close to the emission and height of the emission, Gaussian models generally used to predict the behaviour of atmospheric releases are not well adapted. The study is based on the characterisation of the 85Kr emitted during normal operations of the reprocessing process. Temporal and spatial variations of the plume shape were investigated with intensive in situ measurements. Live in situ techniques to measure the electrons and the photons emitted by the 85Kr have been implemented and will be described. Preliminary results showing the interest of the techniques were presented. Variations of the dose rates created by the photon flux of a plume were directly measured and correlated to other quantities.     

Plutonium isotopes in the lower reaches of the River Rhône over the period 1945-2000: fluxes towards the Mediterranean Sea and sedimentary inventories

Plutonium isotopes in the Rh?ne River originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. Due to a new treatment process applied to the liquid effluents, a decrease of two orders of magnitude in the industrial plutonium discharged into the River Rh?ne has been registered from 1991. Today, 238Pu industrial inputs to the River Rh?ne are still about 10 times higher than those derived from global fallout, while 239+240Pu inputs from industrial and global fallout sources are of similar importance, i.e. 1 GBq y(-1). Our results indicate that the river sedimentary compartment act either as a sink or a delayed-source term of plutonium for the freshwaters depending on the hydraulic regime and flood events. This compartment may then represent an important industrial delayed-source term for the River Rh?ne freshwaters in the coming years as the Marcoule reprocessing plant is being dismantled. These results were obtained from samples collected from the lower course of the River Rh?ne over the 1987-1998 period and analysed for 238Pu and 239+240Pu activities. Both river sedimentary inventories of plutonium isotopes and effective outputs from the River Rh?ne towards the Gulf of Lions have been estimated for each year over the 1945-2000 period. Regarding 239+240Pu, the sedimentary inventory accumulated since 1945 is estimated to be 172+/-35 GBq. If mobile, this amount represents a significant delayed-source term of plutonium on the scale of the Rh?ne watershed.     

A performance estimate for the detection of undeclared nuclear-fuel reprocessing by atmospheric 85Kr

To test the sensitivity of using atmospheric (85)Kr to detect undeclared separation of plutonium from irradiated nuclear-reactor fuel, measurements of atmospheric (85)Kr taken in Tsukuba, Japan are analyzed to determine: (1) a lower limit of detection for discovering anthropogenic (85)Kr emissions, (2) the probability of detecting plutonium separation at the Tokai Reprocessing Plant, and (3) the extent to which these results can be generalized to other sites. A LLD of at least 3.4 sigma=0.14 Bq/m(3) with a theoretical false-positive rate of 0.05% is recommended for safeguards' purposes. At this threshold, the continuous separation of 100, 300, and 900 g equivalent weapon-grade plutonium per day was found to correspond to 10%, 50%, and 80% probability of detection, respectively. The smallest detected concentration was for the continuous separation of 45 g/day, with a probability of detection of about 0.6%. It was found that the detection rate is determined predominantly by the weather.     

Monitoring iodine-129 in air and milk samples collected near the Hanford Site: an investigation of historical iodine monitoring data

While other research has reported on the concentrations of (129)I in the environment surrounding active nuclear fuel reprocessing facilities, there is a shortage of information regarding how the concentrations change once facilities close. At the Hanford Site, the Plutonium-Uranium Extraction (PUREX) chemical separation plant was operating between 1983 and 1990, during which time (129)I concentrations in air and milk were measured. After the cessation of chemical processing, plant emissions decreased 2.5 orders of magnitude over an 8-year period. An evaluation of (129)I and (127)I concentration data in air and milk spanning the PUREX operation and post-closure period was conducted to compare the changes in environmental levels. Measured concentrations over the monitoring period were below the levels that could result in a potential annual human dose greater than 1 mSv. There was a measurable difference in the measured air concentrations of (129)I at different distances from the source, indicating a distinct Hanford fingerprint. Correlations between stack emissions of (129)I and concentrations in air and milk indicate that atmospheric emissions were the major source of (129)I measured in environmental samples. The measured concentrations during PUREX operations were similar to observations made around a fuel reprocessing plant in Germany. After the PUREX Plant stopped operating, (129)I concentration measurements made upwind of Hanford were similar to the results from Seville, Spain.     

Simulating mesoscale transport and diffusion of radioactive noble gases using the Lagrangian particle dispersion model

In order to simulate the impact of mesoscale wind fields and to assess potential capability of atmospheric Lagrangian particle dispersion model (LPDM) as an emergency response model for the decision supports, two different simulations of LPDM with the mesoscale prognostic model MM5 (Mesoscale Model ver. 5) were driven. The first simulation of radioactive noble gas ((85)Kr exponent) emitted during JCO accident occurred from 30 September to 3 October 1999 at Tokai, Japan showed that the first arriving short pulse was found in Tsukuba located at 60km away from the accidental area. However, the released radioactive noble gas was transported back to the origin site about 2 days later due to the mesoscale meteorological wind circulation, enhancing the levels of (85)Kr with the secondary peak in Tsukuba. The second simulation of atmospheric dilution factors (the ratio of concentration to the emission rate, chi/Q), during the underground nuclear test (UNT) performed by North Korea showed that high chi/Q moved to the eastward and extended toward southward in accordance with the mesoscale atmospheric circulations generated by mesoscale prognostic model MM5. In comparison with the measurements, the simulated horizontal distribution patterns of (85)Kr during the JCO are well accord with that of observation in Tsukuba such as the existence of secondary peak which is associated with the mesoscale circulations. However, the simulated level of (85)Kr anomaly was found to be significantly lower than the observations, and some interpretations on these discrepancies were described. Applications of LPDM to two mesoscale emergency response dispersion cases suggest the potential capability of LPDM to be used as a decision support model provided accurate emission rate of accident in case of a large accident.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.     

Carbon-14 transfer into rice plants from a continuous atmospheric source: observations and model predictions

Carbon-14 ((14)C) is one of the most important radionuclides from the perspective of dose estimation due to the nuclear fuel cycle. Ten years of monitoring data on (14)C in airborne emissions, in atmospheric CO(2) and in rice grain collected around the Tokai reprocessing plant (TRP) showed an insignificant radiological effect of the TRP-derived (14)C on the public, but suggested a minor contribution of the TRP-derived (14)C to atmospheric (14)C concentrations, and an influence on (14)C concentrations in rice grain at harvest. This paper also summarizes a modelling exercise (the so-called rice scenario of the IAEA's EMRAS program) in which (14)C concentrations in air and rice predicted with various models using information on (14)C discharge rates, meteorological conditions and so on were compared with observed concentrations. The modelling results showed that simple Gaussian plume models with different assumptions predict monthly averaged (14)C concentrations in air well, even for near-field receptors, and also that specific activity and dynamic models were equally good for the prediction of inter-annual changes in (14)C concentrations in rice grain. The scenario, however, offered little opportunity for comparing the predictive capabilities of these two types of models because the scenario involved a near-chronic release to the atmosphere. A scenario based on an episodic release and short-term, time-dependent observations is needed to establish the overall confidence in the predictions of environmental (14)C models.     

Apparent 85Kr ages of groundwater within the Royal watershed, Maine, USA

Specific 85Kr activity is mapped from 264 domestic and municipal wells sampled during 2002-2004 in the Royal watershed (361 km2), Maine. Gas samples are collected at 20 m, 40 m, and > 50 m interval depths within the unconfined aquifers. Gas extraction for 85Kr from wells is obtained directly via a wellhead methodology avoiding conventional collection of large sample volumes. Atmospheric 85Kr input to the recharge environment is estimated at 1.27 Bq m(-3) by time-series analyses of weighted monthly precipitation (2001-2004). Numerical simulation of Kr gas transport through the variable unsaturated zones to the water table suggests up to 12-year time lags locally, thus biasing the 85Kr groundwater ages. Apparent 85Kr ages suggest that approximately 70% of groundwater near 20 m depth was recharged less than 30 years BP (2004). Mass-age transport modeling suggests that post mid-1950s recharge penetrates to part of the basin's floor and that older groundwater seeps from the underlying fractured bedrock may occur.     

Characteristics of oxidant precursor emissions from anthropogenic sources in the United States

Hydrocarbons (HC) and nitrogen oxides (NO_x) have been identified as the most important precursor pollutants for oxidant formation in the atmosphere. These pollutants are emitted both from natural and anthropogenic sources; however, these two types of sources are generally geographically separated. Anthropogenic emissions are dominant in and around urban centers, where the majority of severe oxidant problems occur. Based on data gathered by the MAP3S/RAINE emissions inventory project, anthropogenic emissions of HC in the conterminous United States were 24.8 million metric tons in 1979. HC emissions were predominantly from area sources, the transportation sector being the largest contributor with 39.8% of the total. State-by-state breakdowns are also included. Based on analyses by other emissions inventory projects, the nonreactive fraction of the emissions from the transportation sector is less than 20% by weight. The highest proportion of HC emissions occur at low altitudes (0–50 m range) in high population density areas. Anthropogenic emissions of NO_x were 23.7 million metric tons in 1979; 50.8% were from point sources. The transportation sector and the electric utilities sector account for 37.1% and 30.9% of the NO_x emissions, respectively. The NO₂ fraction of the emissions from the transportation and electric utilities sectors is less than 10% by weight, based on NO/NO₂ speciation data from two other emissions inventories. Highest rates of NO_x emissions occur in high population density areas and are released at low altitude (0–50 m); three areas of high electric generating capacity were found to have high release altitudes.     

Level and origin of iodine-129 in the Baltic Sea

Environmental samples, such as seawater, seaweed, lake water, lake sediment and grass collected from the Baltic Sea area were analyzed for 129I and 127I by radiochemical neutron activation analysis. In 2000, the concentration of 129I in the seawater from Borholm and M?en in the Baltic Sea has reached 6.0 x 10(-13) and 16 x 10(-13) g/l, respectively, these are more than two orders of magnitude higher than the global fallout level. The highest value of 270 x 10(-13) g/l being found in the seawater from the Kattegat. By comparison of the level of 129I in the lake water and precipitation in this region, it is estimated that more than 95% of 129I in the Baltic Sea originates from reprocessing emissions, especially from the French nuclear fuel reprocessing plant at La Hague. More than 30% of 129I in the south Baltic and 93% in the Kattegat directly originates from the marine discharges of the European reprocessing plants.     

An improved method for Kr analysis by liquid scintillation counting and its application to atmospheric Kr determination

Atmospheric ⁸⁵Kr concentration at Fukuoka, Japan was determined by an improved ⁸⁵Kr analytical method using liquid scintillation counting (LSC). An average value of 1.54 ± 0.05 Bq m⁻³ was observed in 2008, which is about two times that measured in 1981 at Fukuoka, indicating a 29 mBq y⁻¹ rate of increase as an average for these 27 years. The analytical method developed involves collecting Kr from air using activated charcoal at liquid N₂ temperature and purifying it using He at dry ice temperature, followed by Kr separation by gas chromatography. An overall Kr recovery of 76.4 ± 8.1% was achieved when Kr was analyzed in 500-1000 l of air. The Kr isolated by gas chromatography was collected on silica gel in a quartz glass vial cooled to liquid N₂ temperature and the activity of ⁸⁵Kr was measured with a low-background LS counter. The detection limit of ⁸⁵Kr activity by the present analytical method is 0.0015 Bq at a 95% confidence level, including all propagation errors, which is equivalent with ⁸⁵Kr in 1.3 l of the present air under the analytical conditions of 72.1% counting efficiency, 0.1597 cps background count rate, and 76.4% Kr recovery.     

Temporal trends for 99Tc in Norwegian coastal environments and spatial distribution in the Barents Sea

The objective of this study was to reassess 99Tc transit times and transfer factors, from Sellafield to northern Norway, and to determine the extent of 99Tc migration to the Barents Sea. Filtered seawater samples were collected on a monthly basis from Hilles?y, northern Norway, and in February 1999 from the Barents Sea. Results showed an increase in levels of 99Tc at Hilles?y where activity concentrations have increased from a baseline of 0.2-0.4Bq m(-3) to a maximum of 1.6 Bq m(-3). A transit time of 42 months and a transfer factor of 6Bq m(-3) per PBq a(-1) have been derived, using cross-correlation analysis. The current study predicts that future levels are unlikely to increase dramatically over the levels observed in 1998. Levels of 99Tc in the Barents Sea ranged from 0.2 Bq m(-3) to 1.1 Bq m(-3) showing the influence of new 99Tc inputs by early 1999.     

Simulating transport of non-Chernobyl (137)Cs and (90)Sr in the North Atlantic-Arctic region

The spatial and temporal distributions of the anthropogenic radionuclides (137)Cs and (90)Sr, originating from nuclear bomb testing and the Sellafield reprocessing plants in the Irish Sea, are simulated using a global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysed fields for the period 1950 to present. Comparison of temporal evolution of observed and simulated concentrations of (137)Cs have been conducted for the regions east of Scotland, west of central Norway and at the entrance of the Barents Sea. It follows that the radionuclides from the Sellafield discharge reach the Barents Sea region after 4-5 years, in accordance with observations. The simulation provides a detailed distribution and evolution of the radionuclides over the integration time. For the Atlantic waters off the coast of Norway and in the southern Barents Sea, the atmospheric fallout dominates over the Sellafield release up to the mid 1960s and from the early 1990s, whereas Sellafield is the main source for the two radionuclides in the 1970s and 1980s. It is furthermore argued that model systems like the one presented here can be used for future prediction of radioactive contaminations in the Nordic Seas and the Arctic Ocean, for instance under various global warming scenarios.     

The Spanish project on energy and environment: ENMA

The project ENMA assesses the atmospheric pollution caused by the transformation and consumption of energy. The project is in the following stages: (a) estimation of annual overall average emissions; (b) estimation of annual average concentrations of pollutants; and (c) estimation of doses. Estimation of annual overall average emissions is estimated, separately, for urban areas and point sources. Concentrations of pollutants are obtained for urban areas and point-sources by means of two different gaussian models. Finally, doses are calculated assuming that the effects of all pollutants are linear at low doses. Doses for each pollutant, and doses for exposure to several combined pollutants, are defined. The doses on population are also defined, assuming that the significance of pollution depends on the number of people exposed.     

上海市多环芳烃排放清单构建及排放趋势预测

以美国国家环境保护局(US EPA)优先控制污染物清单中16种多环芳烃(PAHs)为研究对象,仅考虑人为排放源,根据11种主要排放源排放数据和相应排放因子估算上海市PAHs年排放量。结果表明:2012年上海市16种PAHs的排放量约为447.8t,7种致癌性PAHs排放量为60.06t,排放密度为70.6kg/km2。从排放源看,炼焦用煤和民用燃煤是PAHs排放的主要来源,两者占总排放量的56.0%,天然气、炼油排放量次之。从排放谱看,萘(NAP)排放量最大,占总量的30.8%,其次为菲(PHE),致癌性PAHs占排放总量的13.4%。另外,PAHs排放以低环(2~3环)为主,占排放总量的71.1%,其次为4环的Fl、Py、BaA和Chr,高环的D[ah]A排放量最低。利用地区生产总值(GDP)和能源消耗数据拟合公式预测2020年能源消耗量,进而预测得2020年PAHs排放量约为356.57t。     

临安区域本底站大气甲烷浓度变化特征

通过分析2006年8月～2009年7月临安区域大气本底站Flask瓶采样获得的CH4浓度特征,结合地面风向、后向轨迹、排放清单,研究了CH4浓度变化特征和长三角地区排放源对CH4浓度的影响作用。结果表明,临安区域大气本底站的CH4浓度分布在1 7584×10-9~1 9700×10-9,具有较明显的季节波动变化特征,浓度季节变化幅度为737×10-9;CH4浓度平均年增幅达176×10-9,增速较快。东北风和东南风时,CH4浓度较高;西南风时CH4浓度较低。导致CH4高浓度分布的气团主要来自临安站的东北、偏东方向;导致CH4低浓度分布的气团集中在西南 偏南     

Relict communities and populations of petrophilous plant species in northern regions of Sverdlovsk oblast and problems in their conservation

An inventory of rock vegetation has been taken in river valleys on the eastern slope of the southern part of the Northern Urals and the northern part of the Middle Urals. New habitats of some rare plant species, relict communities of forest-steppe species at the northern limit of their distribution, and ultrasmall populations of petrophilous species growing in isolation for a long time have been revealed. In studies on a group of similar specially protected areas (e.g., within river valleys), it is proposed to identify key sites distinguished by the highest species richness of vegetation     

85Kr atmospheric concentration in Bratislava from 1980 to 1983

A cryogenic-chromatographic method for determination of ⁸⁵Kr in the atmosphere is presented. Sampling of the air on the activated-charcoal, chromatographic separation of Krypton from the other air components and radioactivity measurement are described in details. The activity of ⁸⁵Kr is measured by small proportional counters with sensitive volumes of 5 and 10 cm³. Results of the measurements of ⁸⁵Kr air concentration in Bratislava from 1980 to 1983 are presented and compared with other ⁸⁵Kr data measured in Europe.