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1.
In October 1957 a fire in Pile Number 1, a nuclear reactor at the Windscale Works, Sellafield, resulted in the accidental release of radionuclides to the atmosphere. Previous studies have described the atmospheric transport of the resultant radioactive plume from its release on the Cumbrian coast of Northwest England to its passage across mainland Europe. Those past studies have suffered from uncertainties concerning the quantity and timing of emissions and meteorological conditions. Crabtree [1959. The travel and diffusion of the radioactive material emitted during the Windscale accident. Quarterly Journal of the Royal Meteorological Society 85, 362] initially produced estimates of plume transport based on weather observations and radiosonde profiles. Later, ApSimon et al. [1985. Long-range atmospheric dispersion of radioisotopes—I. The MESOS model. Atmospheric Environment 19(1), 99–111] based estimates of plume transport on trajectories calculated from weather charts. More recently, Nelson et al. [2006. A study of the movement of radioactive material discharged during the Windscale fire in October 1957. Atmospheric Environment, 40, 58–75] used a full three-dimensional dispersion model using digitised weather data from similar charts.This study aims to further reduce uncertainty in the plume's behaviour by using the latest available Numerical Weather Prediction Model reanalysis of meteorological data from the European Centre for Medium Range Weather Forecasts (ERA-40) coupled with current best estimates of the radioactive emissions profile. The results presented here generally support the findings of previous studies though an improvement in model comparisons against observational measurements has been found. The opportunity was also taken to extend the time horizon, and hence geographical coverage, of the modelled plume. It is considered that this paper presents the best estimate to date of the plume's behaviour.  相似文献   

2.
Several environmental media in Austria were monitored for artificial radionuclides released during the Fukushima nuclear accident. Air (up to 1.2 mBq/m3 particulate 131I) and rainwater (up to 5.2 Bq/L 131I) proved to be the media best suited for the environmental monitoring, allowing also a temporal resolution of the activity levels. Significant regional differences in the wet deposition of 131I with rain could be observed within the city of Vienna during the arrival of the contaminated air masses. Forward-trajectory analysis supported the hypothesis that the contaminated air masses coming from the northwest changed direction to northeast over Northern Austria, leading to a strong activity concentration gradient over Vienna. In the course of the environmental monitoring of the Fukushima releases, this phenomenon—significant differences of 131I activity concentrations in rainwater on a narrow local scale (8.1 km)—appears to be unique. Vegetation (grass) was contaminated with 131I and/or 137Cs at a low level. Soil (up to 22 Bq/kg 137Cs) was only affected by previous releases (nuclear weapon tests, Chernobyl). Here, also significant local differences can be observed due to different deposition rates during the Chernobyl accident. The effective ecological half-lives of 137Cs in soil were calculated for four locations in Austria. They range from 7 to 30 years. No Austrian sample investigated herein exceeded the detection limit for 134Cs; hence, the Fukushima nuclear accident did not contribute significantly to the total radiocesium inventory in Austrian environmental media. The levels of detected radioactivity were of no concern for public health.  相似文献   

3.
Leaves of linden (Tilia tomentosa L. and Tilia cordata Mill.) and horse chestnut (Aesculus hippocastanum L.) were analysed as biomonitors of radionuclides in urban air. Samples of soils, leaves and aerosols were collected in Belgrade, Serbia. Activities of 137Cs, 40K, 210Pb and 7Be in the samples were measured on an HPGe detector by standard gamma spectrometry. “Soil-to-leaves” transfer factors were calculated. Student’s t test and linear Pearson correlation coefficients were used for statistical analysis. Differences in local conditions at the sampling sites were not significant, and the mechanisms of the radionuclides’ accumulation in both plant species are similar. Ceasium-137 was detected in some of the leaf samples only. Transfer factors for 137Cs and 40K were (0.03–0.08) and 1.3, respectively. The concentrations of 210Pb and 7Be in leaves were higher in autumn than in spring, and there were some similarities in their seasonal patterns in leaves and in air. Weak to medium correlation was obtained for the 210Pb and 7Be activities in leaves and aerosols. Large positive correlation was obtained for the 210Pb activities in linden leaves and the mean activity in aerosols for the preceding months. Different primary modes of radionuclides accumulation in leaves were observed. Since large positive correlation was obtained for the 210Pb activity in linden leaves and the mean in aerosols for the preceding months, mature linden leaves could be used as biomonitors of recent 210Pb activity in air.  相似文献   

4.
The presence of cesium-137 (137Cs) in the environment is mainly due to past nuclear tests and accidental reactor releases. Due to the half-life of 137Cs (30.2 y), amounts of this radionuclide releases are in fact still detectable in soils, and at trace levels in the vegetation and the atmosphere. Since the middle of the 1990’s, the presence of 137Cs in the atmosphere has long been attributed to the resuspension of terrestrial dust. Recently, modelling studies have demonstrated that an additional and possibly dominant source of this anthropogenic radionuclide is biomass burning. Here, we report the variations of atmospheric 137Cs activity levels over a 2-year period at the puy de Dôme (1465 m a.s.l.), France in combination with measurements of the aerosol chemical composition, in particular with indicators for biomass burning (levoglucosan and potassium) and soil dust (calcium). Temporal co-variations of these chemical compounds in addition to back-trajectories are used to identify common source emissions. Significant correlation is found between these compounds. Hence, we experimentally confirm the modelling study highlighting the fact that the atmospheric 137Cs is partly released by biomass burning. In addition, we observed that the correlations between the 137Cs concentrations and levoglucosan and biomass burning K+ differ according to the season. This is in agreement with the temporal evolution of levoglucosan concentration, which has maxima in winter and minima in summer.  相似文献   

5.
ABSTRACT

To facilitate routine health risk assessments, we develop the concept of an inhalation transfer factor (ITF). The ITF is defined as the pollutant mass inhaled by an exposed individual per unit pollutant mass emitted from an air pollution source. A cumulative population inhalation transfer factor (PITF) is also defined to describe the total fraction of an emitted pollutant inhaled by all members of the exposed population. In this paper, ITFs and PITFs are calculated for outdoor releases from area, point, and line sources, indoor releases in single zone and multizone indoor environments, and releases within motor vehicles. Typical PITFs for an urban area from emissions outdoors are ~10-6–10-3. PITFs associated with emissions in buildings or in moving vehicles are typically much higher, ~10-3–10-1.  相似文献   

6.
Artificial radionuclides, such as iodine-131 (131I), cesium-134 (134Cs), and cesium-137 (137Cs), as well as natural isotopes of beryllium-7 (7Be) and potassium-40 (40K) have been registered in atmospheric aerosols over Vladivostok selected from 11 March to 17 June 2011. Additionally, 134Cs and 137Cs were detected in atmospheric aerosols over Tomsk selected from 16 March to 17 June 2011. Artificial radionuclides were also discovered in atmospheric wet depositions sampled in Vladivostok from 3 to 17 May 2011. Moreover, these radionuclides have been registered in atmospheric aerosols over the sea surface of the Sea of Japan selected from 3 to 31 May 2011 during an expedition of the “Nadezhda” sailing ship. From 18 March to 15 April, an increase in concentrations of atmospheric aerosols over Vladivostok from 108.8 to 321.5 μg/m3 has been registered. It was accompanied by increased activity concentrations of 134Cs, 137Cs, and the 131I. During the period from 18 March to 15 April, activity concentrations of 137Cs and 134Cs in atmospheric aerosols increased 100 times compared with the minimum detectable concentration (MDC) level and peaked in the weekly sample gathered from 8 to 15 April (145.0 and 105.3 μBq/m3, respectively). Variability of concentrations of natural isotopes of 7Be and 40K was not greater than 1 order of magnitude throughout the sampling period. Maximal values of 137Cs and 134Cs concentrations (1,281.5?±?141 and 384.4?±?42.3 μBq/m3, respectively) in Tomsk were reached in samples taken from 1 to 2 April. For the atmospheric aerosol samples from the Sea of Japan, the largest concentration of 131I (392.3?±?215.7 μBq/m3) was detected from 13 to 19 May, while all other samples had much lower concentration values. Synoptic analysis of back trajectories movement of air masses showed that the radioactive cloud came to Vladivostok from the regions of Siberia and northeastern part of China. Synoptic analysis for Tomsk showed that during the period of maximal activity concentrations (1–9 April), air masses were arriving from the European part of Russia and north of Kazakhstan.  相似文献   

7.
The nuclear accident at the Fukushima Daiichi Nuclear Power Plant (FDNPP) which occurred after the Great East Japan Earthquake on March 11, 2011 resulted in releases of radionuclides such as 134Cs (half-life:T1/2 = 2.06 yr), 137Cs (T1/2 = 30.04 yr) and 131I (T1/2 = 8.05 d) to the environment. For this paper, we observed the monthly variations of radiocesium (134Cs and 137Cs) and stable Cs concentrations in influent, effluent, sewage sludge, and sludge ash collected from a sewage treatment plant 280 km north of the FDNPP from July to December, 2011. Using the stable Cs results, we concluded the mass balance of Cs in the sewage treatment plant showed that about 10% of the Cs entering the sewage treatment plant would be transferred to the sewage sludge, and then Cs in the sewage sludge was totally recovered in the sludge ash. The behavior of Cs was similar to that of Rb, but it was not similar to that of K in the sewage treatment process.  相似文献   

8.
Results are reported for a series of migration experiments performed in a hydraulically characterized, single, natural fracture in a block of granite with overall dimensions of 1 × 1 × 0.7 m (all approximate), using the conservative, poorly sorbing and strongly sorbing radionuclides 3H20, 131I, 22Na, 85Sr, 137Cs, 60Co, 154,155Eu, 237Np, and 238Pu. The volumetric flow velocity of the transport solution was 3 ml h−1, giving a residence time in the fracture of approximately 50 h. Elution profiles were obtained for 3H20, 131I, 22Na, 85Sr and 137Cs but no evidence of the other radionuclides was observed in the eluent. Results from supporting static sorption measurements on crushed geological materials and granite coupons showed in general higher sorption on alteration minerals than on granite. Sorption was lowest for 22Na and 85Sr.The migration of 131I, 22Na, 85Sr through the fracture in real time was followed using end-window Geiger-Müller probes located in unused boreholes. Additional information, obtained by alpha and gamma scanning of the fracture surfaces after separating the block along the fracture, confirmed that transport had occurred along the flow path predicted from the hydraulic characterization of the fracture and that, over a 5.5 month period, the bulk of the injected 137Cs had migrated only 75 cm along the flow path. The 60Co, the rare earths and the actinides had not moved beyond the location of the injection borehole, suggesting that fracture infilling minerals played a major role in retarding radionuclide transport. Additional confirmation of the role of secondary minerals in radionuclide retardation was obtained using selective sequential extraction on the fracture surfaces. These observations support the inclusion of sorption data for fracture infilling minerals in the sorption database developed for the geosphere model for the Canadian Nuclear Fuel Waste Management Program.  相似文献   

9.
Single-particle mass spectrometry data collected during the Pittsburgh Supersite experiment was used to isolate an episode on 27 October 2001 when the measurement site was primarily influenced by emissions from coal combustion sources. Results showed that (a) 60–80% of the particles detected during this event belonged to the Na/Si/K/Ca/Fe/Ga/Pb particle class associated with coal combustion emissions, (b) observation of this class was an isolated event occurring only during the hours of 06:00–14:00 EST, and (c) the detection of these particles was highly correlated with shifts in wind direction. Coincident SMPS, TEOM PM2.5, SO2, NOx, and O3 measurements were in excellent agreement with the single-particle results in terms of both identifying and characterizing this event. The three most likely point sources of these particles were isolated and Gaussian plume dispersion models were used in reverse to predict their particle number, particle mass, and gas phase emissions. Calculated mass emission rates were in general agreement with the US EPA National Emissions Inventory (NEI) database emissions estimates and the Title V PM10 limit. The largest of the three sources emits about 2.4×1017 fine and ultrafine particles per second.  相似文献   

10.
The present study focuses on the exceptional Saharan dust event that affected most of France in February 2004. Activity levels of various artificial radionuclides (90Sr, 137Cs, uranium, thorium and plutonium isotopes, 241Am) were examined. Activity or isotopic ratios are discussed in the context of atmospheric nuclear weapons tests, among them French tests performed in Sahara in the 1960s. The daily evolution of 137Cs activity levels in the atmosphere was compared to daily PM10 change. A link between airborne 137Cs and PM10, is given. It is estimated that this 2-day event deposited as much 137Cs as would be deposited on average over a 10-month period. The amount of deposited 137Cs and 239+240Pu represents respectively about 0.1 and 1% of the activity already present in the soil. Such Saharan dust events correspond to an extreme type of “feeder” process of artificial radionuclides in the atmosphere. Therefore, they contribute to the long term background level of artificial radionuclides kept at trace levels in the atmosphere.  相似文献   

11.
Radionuclide concentration analysis of total moss bodies often gave relatively different results than a separate analysis of each different morphological part of the same sample. The dynamics of the transfer of metals by dust uplifted from the soil and another approach, based on the diffusion of the two radionuclides to the moss, have been analyzed. In the proposed model, short- and long-term approaches have been applied. Each part of a moss’s profile can show different radionuclides accumulation ability, including both 210Pb and 210Po isotopes. A first-order kinetic model has been used for 210Po and 210Pb transport between three body components of mosses. This mathematical approach has been applied for 210Po activity concentration in the air estimation. For relatively clean deep forest region, calculated concentrations were from 17.2 to 43.8 μBqm?3, while for urban air concentrations were higher from 49.1 to 104.9 μBqm?3.  相似文献   

12.
《Chemosphere》2002,49(10)
The distribution coefficients (Kd) and desorption rates of 137Cs and 241Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The Kd values were found to be 500 for 137Cs and 3800 for 241Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for 137Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of 137Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of 241Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the 241Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than 137Cs under Black Sea conditions.  相似文献   

13.
The influence of ship emissions on ozone (O3) concentrations in a coastal area (CA) including Busan port, Korea was examined based on a numerical modeling approach during a high O3 episode. The analysis was performed by two sets of simulation scenarios: (1) with ship emissions (e.g., TOTAL case) and (2) without ship emissions (e.g., BASE case). A process analysis (PA) (the integrated processes rate (IPR) and integrated reaction rate (IRR) analyses) was used to evaluate the relative contributions of individual physical and chemical processes in O3 production in and around the CA (e.g., sites of Dong Sam (DS) and Dae Yeon (DY)). The model study suggested the possibility that pollutant gases emitted from the ships traversing Busan port can exert a direct impact on the O3 concentration levels in the CA. Largest impacts of ship emissions on the O3 concentrations were predicted at the coast (up to 15 ppb) and at inland locations (about 5 ppb) due to both the photochemical production of pollutant gases emitted from the ships and meteorological conditions. From the PA, the photochemical production of O3 (P(O3)) due to ship emissions in the CA was found to increase by a mean of 1.5 ppb h?1 (especially by ≥10 ppb h?1 at the DS site) during the day.  相似文献   

14.
Abstract

Mercury-bearing material enters municipal landfills from a wide array of sources, including fluorescent lights, batteries, electrical switches, thermometers, and general waste; however, the fate of mercury (Hg) in landfills has not been widely studied. Using automated flux chambers and downwind atmospheric sampling, we quantified the primary pathways of Hg vapor releases to the atmosphere at six municipal landfill operations in Florida. These pathways included landfill gas (LFG) releases from active vent systems, passive emissions from landfill surface covers, and emissions from daily activities at each working face (WF). We spiked the WF at two sites with known Hg sources; these were readily detected downwind, and were used to test our emission modeling approaches. Gaseous elemental mercury (Hg0) was released to the atmosphere at readily detectable rates from all sources measured; rates ranged from ~1–10 ng m?2 hr?1 over aged landfill cover, from ~8–20 mg/hr from LFG flares (LFG included Hg0 at μg/m3 concentrations), and from ~200–400 mg/hr at the WF. These fluxes exceed our earlier published estimates. Attempts to identify specific Hg sources in excavated and sorted waste indicated few readily identifiable sources; because of effective mixing and diffusion of Hg0, the entire waste mass acts as a source. We estimate that atmospheric Hg releases from municipal landfill operations in the state of Florida are on the order of 10–50 kg/yr, substantially larger than our original estimates, but still a small fraction of current overall anthropogenic losses.  相似文献   

15.
We present bioaerosol source term concentrations from passive and active composting sources and compare emissions from green waste compost aged 1, 2, 4, 6, 8, 12 and 16 weeks. Results reveal that the age of compost has little effect on the bioaerosol concentrations emitted for passive windrow sources. However emissions from turning compost during the early stages may be higher than during the later stages of the composting process. The bioaerosol emissions from passive sources were in the range of 103–104 cfu m−3, with releases from active sources typically 1-log higher. We propose improvements to current risk assessment methodologies by examining emission rates and the differences between two air dispersion models for the prediction of downwind bioaerosol concentrations at off-site points of exposure. The SCREEN3 model provides a more precautionary estimate of the source depletion curves of bioaerosol emissions in comparison to ADMS 3.3. The results from both models predict that bioaerosol concentrations decrease to below typical background concentrations before 250 m, the distance at which the regulator in England and Wales may require a risk assessment to be completed.  相似文献   

16.
Methane (CH4) is an important greenhouse gas that is predominantly emitted to the atmosphere from anoxic wetland ecosystems. Understanding the sources and emissions of CH4 is crucially important for climate change predictions; however, there are significant discrepancies between CH4 source estimates derived via so-called bottom-up and top-down methods. Here we report CH4 emission from the stems of mature wetland alder (Alnus glutinosa) trees in the UK, a common tree of northern hemisphere floodplains and wetlands. The alder stems most likely behave as conduits for soil-produced CH4 either in the gaseous or aqueous phase, and may, therefore, help to reconcile methodological differences in the way the wetland CH4 source is estimated.Alder tree stems emitted average peak CH4 fluxes of 101 μg CH4 m?2 h?1 (on a stem area basis) in early October, a rate that is similar to that obtained from mature Japanese ash (Fraxinus mandshurica var. japonica) in Japan and amounting to approximately 20% of the measured CH4 flux from the soil surface. The finding suggests that trees, which occupy 60% of Earth's wetlands and are normally excluded from the measurement programmes that form the basis for bottom-up estimates of the global wetland source, could be important contributors to overall terrestrial ecosystem CH4 flux.  相似文献   

17.
Activity concentrations, inventories and activity ratios of 137Cs, 238Pu, 239?+?240Pu and 241Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m2 for 137Cs, 238Pu, 239?+?240Pu and 241Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The 238Pu/239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The 238Pu/239?+?240Pu and 239?+?240Pu/137Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.  相似文献   

18.
Decades-long monitoring of anthropogenic radionuclides in the atmospheric deposition in Tsukuba, Japan suggests not only the substantial impacts of the Asian dust (Kosa) on the deposition but also the possible change of the Kosa source region, especially during springs of the 2000s. In order to know more about such change, 4 single wet deposition events occurred in the spring of 2007 were scrutinized. The largest anthropogenic radionuclides wet deposition was supplied by the April 2–4 event. It brought several tens % of the monthly depositions (April 2007) of the dust (residue) mass (4.5 g m?2) and anthropogenic radionulides (90Sr: 16, 137Cs: 97 and Pu: 3 mBq m?2). None of the events observed fulfilled both criteria of the specific activities and 90Sr/137Cs activity ratio to the Tsukuba soil; they did not exhibit local soil dust signature. The Kosa events in fact have extensive impacts on the atmospheric environment over Japan in spring season. Considering the elevated specific activities as well as greater 137Cs/90Sr activity ratio in the deposited dust, it is hypothesized that the dust source areas in Asian continent would be shifting from the arid zone to the desert-steppe zone suffering from desertification during the 2000s. This type of the Kosa may be called as the ‘new-regime Kosa’. Chemical observation in the far downwind region of the Kosa dust could allow us to know possible shift in the source regions.  相似文献   

19.
Particle number size distribution data in the range from 0.015 to 0.630 μm were collected over a 5-year period in the central business district (CBD) of Brisbane, Australia. Particle size distribution was summarised by total number concentration and number median diameter (NMD) as well as the number concentration of the 0.015–0.030 (N15–30), 0.030–0.050 (N30–50), 0.050–0.100 (N50–100), 0.100–0.300 (N100–300) and 0.300–0.630 (N300–630) μm size classes. Morning (6:00–10:00) and afternoon (16:00–19:00) measurements, the former representing fresh traffic emissions (based on the local meteorological conditions) and the latter well-mixed emissions from the CBD, during weekdays were extracted and the respective monthly mean values were estimated for time series analysis. For all size fractions, average morning concentrations were about 1.5 higher than in the afternoon whereas NMD did not vary between the morning and afternoon. The trend and seasonal components were extracted through weighted linear regression models, using the monthly variance as weights. Only the morning measurements exhibited significant trends. During this time of the day, total particle number increased by 105.7% and the increase was greater for larger particles, resulting in a shift in NMD by 7.9%. Although no seasonal component was detected the evidence against it remained weak due to the limitations of the database.  相似文献   

20.
Accidental releases of waste water from the first Czechoslovak nuclear power plant, A1, caused contamination of sediments of the Dudváh river, flowing into the Vah river, in Slovakia. Rather high concentrations of 137Cs and 90Sr (2150Bq dm−3 and 215Bq dm−3, respectively) were found in bottom sediments of a former channel of the re-engineered river body at a distance of about 250 m from a village, Siladice, with water-supply wells. In order to assess the possibility of contamination of the wells, underground migration of both radionuclides from the contaminated area was simulated using an original layered convection-diffusion model. Kd values determined in laboratory experiments were used. The analysis of the hydrological situation in the area reveals that the critical condition is a dominant horizontal groundwater flow near the water table in the direction from the Váh bank to Siladice, in the periods when the contaminated body lies under the water table. The simulation calculated under conservative conditions showed that the contamination of water-supply wells would not exceed permissible concentration limits.  相似文献   

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