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1.
Experimental field and laboratory studies on washout of radionuclides from the snow cover during snow melting were carried out in the winter of 2005/06. In the field studies, a specially equipped runoff site was used. In the laboratory conditions, the experiments were conducted using prepared soil monoliths. In the winter of 2006, 25 g/m2 of water-free cesium chloride (CsCl) and 25 g/m3 of strontium chloride (SrCl2) were put onto the snow cover surface of the runoff site. The snow surface of the soil monolith was coated with a 137Cs-bearing solution, then with SrCl2. Under experimental conditions, practically no surface runoff from the runoff site was recorded. The experiments with the soil monoliths demonstrated that the coefficient of the liquid washout of 137Cs normalized to the runoff layer was within 0.9 × 10?6–1.2 × 10?4 mm?1, and that of 90Sr normalized to the runoff layer was within 2 × 10?–1.6 × 10?4 mm?1.  相似文献   

2.
The series of δ18O values is presented for all precipitation events in Moscow in 2014. Precipitation samples were taken at the observation site of the Meteorological Observatory of Lomonosov Moscow State University (MSU MO), and the isotopic analysis was carried out in the isotopic laboratory of the Department of Geography of MSU. The concentration of stable 18O in precipitation over Moscow in 2014 varied from -0.09 to -26.29‰. The maximum amplitudes of δ18O were registered in March-April and October. The pronounced interrelation was revealed between the oxygen isotopic composition of precipitation and surface air temperature (the correlation coefficient is 0.85). The computation of back trajectories of air masses and the analysis of weather charts demonstrated that the most isotopically light precipitation is typical of relatively cold air masses slowly moving over the continent during the last five days before precipitation. In this case, the ongoing condensation leads to the progressive isotopic depletion of precipitation (more and more isotope-depleted precipitation is registered). On the contrary, fast air transport from the middle and even from high latitudes of the Atlantic Ocean leads to the relatively constant of δ18O values of precipitation.  相似文献   

3.
The estimate of the release of radioactive substances (133Xe, 131I, and 137Cs) into the atmosphere from the Fukushima Daiichi nuclear disaster is presented. It was obtained using the FLEXPART Lagrangian dispersion model and the data of local ground-based measurements of radiation dose rate. The computation period covers the active phase of the nuclear disaster that lasted 20 days after the tsunami. To get the quantitative characteristics of emissions of radioactive substances, the inverse modeling based on the Bayesian approach is used. The emissions were estimated for three altitudes. The total emissions are equal to 2.1 + 0.4 kg (14 000 + 2700 PBq) for 133Xe, (3.8 + 0.4) x 10-2 kg (174 + + 18 PBq) for 131I, and 5.7 + 1.2 kg (18 + 4 PBq) for 137Cs that is consistent with the results of other studies. Retrieved emissions were used to provide the forward modeling for mapping the areas of radionuclide deposition. The developed method of retrieving the emission of radioactive substances makes a useful instrument that operationally estimates and localizes the areas of potential pollution in case of nuclear accidents and could be used for making decisions on the population evacuation.  相似文献   

4.
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5.
90Sr runoff amounted to 0.22–0.67% of its budget in the catchment; the value is lower for high-latitude rivers running in the zone of frozen and seasonally frozen grounds. The ecological half-period of a decrease in the 90Sr concentration in the river water of Eastern Fennoscandia amounted to 5.9–11.5 years in 1979–1985. The lake waters (Lake Ladoga and Lake Päijänne) were renewed approximately 4–5 times faster than the 90Sr content decreased in these lakes.  相似文献   

6.
The carbon kinetic isotope effects (KIEs) in the reactions of several unsaturated hydrocarbons with chlorine atoms were measured at room temperature and ambient pressure using gas chromatography combustion isotope ratio mass spectrometry (GCC-IRMS). All measured KIEs, defined as the ratio of the rate constants for the unlabeled and labeled hydrocarbon reaction k 12/k 13, are greater than unity or normal KIEs. The KIEs, reported in per mil according to Cl ɛ = (k 12/k 13−1) × 1000‰ with the number of experimental determinations in parenthesis, are as follows: ethene, 5.65 ± 0.34 (1); propene, 5.56 ± 0.18 (2); 1-butene, 5.93 ± 1.16 (1); 1-pentene, 4.86 ± 0.63 (1); cyclopentene, 3.75 ± 0.14 (1); toluene, 2.89 ± 0.31 (2); ethylbenzene, 2.17 ± 0.17 (2); o-xylene, 1.85 ± 0.54 (2). To our knowledge, these are the first reported KIE measurements for reactions of unsaturated NMHC with Cl atoms. Relative rate constants were determined concurrently to the KIE measurements. For the reactions of cyclopentene and ethylbenzene with Cl atoms, no rate constant has been reported in refereed literature. Our measured rate constants are: cyclopentene (7.32 ± 0.88) relative to propene (2.68 ± 0.32); ethylbenzene (1.15 ± 0.04) relative to o-xylene (1.35 ± 0.21), all × 10−10 cm3 molecule−1 s−1. The KIEs in reactions of aromatic hydrocarbons with Cl atoms are similar to previously reported KIEs in Cl-reactions of alkanes with the same numbers of carbon atoms. Unlike the KIEs for previously studied gas-phase hydrocarbon reactions, the KIEs for alkene–Cl reactions do not exhibit a simple inverse dependence on carbon number. This can be explained by competing contributions of normal and inverse isotope effects of individual steps in the reaction mechanism. Implications for the symmetries of the transition state structures in these reactions and the potential relevance of Cl-atom reactions on stable carbon isotope ratios of atmospheric NMHC are discussed.  相似文献   

7.
The issues of assessing variability of 137Cs fallout of global and Chernobyl origin at reference sites are discussed with a purpose to use this isotope as a tracer for estimating the rates of erosion-accumulative processes. It is shown that local variability of soil contamination by 137Cs at reference sites is within 7–20%, which makes it possible to use the isotope as a tracer. When studies are conducted within drainage basins, the available trend of the atmospheric 137Cs fallout should be taken into account in assessing the soil and sedimentation redistribution.  相似文献   

8.
The estimates of 137Cs emissions from the accident happened in Elektrostal at the beginning of April 12, 2013 are presented. The transport of radionuclides and their dry and wet deposition on the surface are computed using the Lagrangian stochastic model of the NOSTRADAMUS software package worked out by Nuclear Safety Institute of Russian Academy of Sciences. Prognostic fields of wind (horizontal and vertical components) in the lower troposphere, precipitation, and vertical and horizontal turbulence diffusivity coefficients in the lower atmosphere (up to 4 km) were used as input data. Prognostic fields were obtained using the WRF-ARW numerical mesoscale model.  相似文献   

9.
The analysis of possible mechanisms of 137Cs concentration changes in surface waters was performed in the process of preparation of reliable long-range forecasts of radioactive river contamination after the Chernobyl accident. The following mechanisms were considered: (1) radioactive decay; (2) advective transport with river waters; (3) irreversible sorption; (4) vertical migration deep into bottom sediments due to diffusion; (5) burial in clean bottom sediments. The data published on 137Cs monitoring at Dobrush, on the Iput’ River in Belarus were used in the analysis. It is shown that the best agreement with the experimental results is achieved when the second, third, and fifth mechanisms are used in calculations. However, a dominating mechanism still cannot be chosen at the present stage of our study. Most probably, all of these mechanisms act simultaneously.  相似文献   

10.
Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10?13 cm3 molecule?1 s?1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10?13 cm3 molecule?1 s?1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/? 0.8 nmol m?2 d?1 for CH2I2 and 3.7 +/? 0.8 nmol m?2 d?1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10?13 cm3 molecule?1 s?1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.  相似文献   

11.
With the aim to achieve quantitative monitoring of sand-dust storms in real time, wind-profiling radar is applied to monitor and study the process of four sand-dust storms in the Tazhong area of the Taklimakan Desert. Through evaluation and analysis of the spatial-temporal distribution of reflectivity factor, it is found that reflectivity factor ranges from 2 to 18 dBz under sand-dust storm weather. Using echo power spectrum of radar vertical beams, sand-dust particle spectrum and sand-dust mass concentration at the altitude of 600 ～ 1500 m are retrieved. This study shows that sand-dust mass concentration reaches 700?μg/m3 under blowing sand weather, 2000?μg/m3 under sand-dust storm weather, and 400?μg/m3 under floating dust weather. The following equations are established to represent the relationship between the reflectivity factor and sand-dust mass concentration: Z?=?20713.5?M 0.995 under floating dust weather, Z?=?22988.3?M 1.006 under blowing sand weather, and Z?=?24584.2?M 1.013 under sand-dust storm weather. The retrieval results from this paper are almost consistent with previous monitoring results achieved by former researchers; thus, it is implied that wind-profiling radar can be used as a new reference device to quantitatively monitor sand-dust storms.  相似文献   

12.
Chernobyl radioactivity in precipitation was measured at Tsukuba, Japan, as were both surface-air concentrations and particle-size distributions of Chernobyl-released radionuclides. To understand the wet removal processes of the Chernobyl radionuclides, i.e.137Cs,103Ru, and90Sr, wet deposition velocities were calculated. The wet deposition velocities of the Chernobyl radioactivity for individual rainfall events varied largely. The wet deposition velocity is given as the product of washout ratio and rainfall rate. Typically, it was found that the washout ratios of90Sr are systematically larger than those of137Cs. In order to explain this fact, we examined the relationship between the washout ratios and particle sizes of radionuclide-bearing aerosols. A positive correlation between corrected washout ratios and particle size was found with a particle diameter range from 0.35 to 1.2 µm. The result strongly suggests that the factors controlling the wet removal of the Chernobyl radioactivity for individual rainfall events are surface air concentration, particle size, and rainfall rate, rather than precipitation amount, which is in agreement with previous understandings. This suggests that high contamination areas of radioactivity are formed during heavy rainfall events with high rainfall rates in the case of tropospheric injection such as the Chernobyl accident.  相似文献   

13.
Using a single drop experiment, the uptake of NO3 radicals on aqueous solutions of the dye Alizarin Red S and NaCl was measured at 293 K. Uptake coefficients in the range (1.7–3.1) ⋅ 10− 3 were measured on Alizarin Red S solutions. The uptake coefficients measured on NaCl solutions were in the range of (1.1–2.0) ⋅ 10−3 depending on the salt concentration. Both experiments lead to a consistent result for the mass accommodation coefficient of αNO3 = (4.2− 1.7+2.2)⋅ 10−3. The product H(Dl kCl−II)0.5 for the NO3 radical was determined to be (1.9 ± 0.2) M atm− 1 cm s−0.5 M−0.5 s−0.5 by fitting the uptake data for the NaCl solutions to the so-called resistance model. The yield of the chemical NO3 radical source was characterized using UV-VIS and FT-IR spectroscopy. The amount of gas-phase NO3 radicals measured at elevated humidities was less than expected. Instead, a rise of the gas-phase HNO3 concentration was found indicating a conversion of gas-phase NO3 radicals to gas-phase HNO3 on the moist reactor walls.  相似文献   

14.
The results of research of diurnal and seasonal dynamics of CO2 emission from the oligotrophic swamp surface in the southern taiga subzone of Western Siberia in 2005–2007 are under consideration. During the summertime, the intensity of CO2 emission increases from spring to the midsummer and then decreases by the fall. A mean CO2 emission value was 118 mg CO2/(m2 hour). The analysis of diurnal dynamics of CO2 emission showed that the maximum CO2 flux is observed at 16:00, while the minimum, at 07:00. Mean amplitude of diurnal variations of the CO2 emission is 74 mg CO2/(m2 hour). The relations established between air temperature and CO2 flux allowed calculating carbon dioxide emission for the periods between measurements. It was found that in the summertime, the period between 10:00 and 13:00 was optimal for measuring CO2 emission with a chamber method.  相似文献   

15.
The heterogeneous interaction of nitrogen dioxide with ammonium chloride was investigated in a molecular diffusion tube experiment at 295–335 K and interpreted using Monte Carlo trajectory calculations. The surface residence time (τsurf) of NO2 on NH4Cl is equal to 15 μs at 295 K, increases with temperature up to 323 K (τsurf = 45 μs) and probably decreases beyond 323 K. The same experiment also yields uptake coefficients, γ, which are derived from the absolute number of surviving molecules effusing out of the diffusion tube. The rate of uptake of NO2 on NH4Cl followed a rate law first order in [NO2] and the uptake coefficient γ is equal to 7 × 10−5 at 295 K, increases with temperature up to 323 K (γ = 2.1 × 10−4) and probably decreases beyond 323 K. Nitrous acid, water and nitrogen were detected as products. From these products, it is concluded that the reaction of NO2 with NH4Cl is a reverse disproportionation reaction where two moles of NO2 result in ammonium nitrite, NH4NO2, as an intermediate, and nitryl chloride, NO2Cl. NH4NO2 decomposes in two pathways, one to nitrous acid, HONO and NH3, the other to nitrogen and water. The branching ratio for the production of HONO + NH3 to that of N2 + H2O is approximately 20 at 298 K and increases with increasing temperature.  相似文献   

16.
To characterize atmospheric particulate matter equal or less than 2.5 μm in diameter (PM2.5) over the Tropical Atlantic Ocean, aerosol sampling was carried out in Puerto Rico during August and September, 2006. Aerosols were analyzed by ion chromatography for water-soluble inorganic and organic ions (including Na+, NH4 +, Mg2+, Ca2+, K+, Cl?, SO4 2?, NH4 +, F?, methanesulfonate (MSA), and oxalate), by inductive coupled plasma mass spectrometry (ICPMS) for trace elements (Al, Fe, Zn, Mn, Cu, Ni, V, Pb, Cr, Sb, Co, Sc, Cd), and by scanning electron microscopy for individual aerosol particle composition and morphology. The results show that the dominant cations in aerosols were Na+, (mean: 631 ng m?3), accounting for 63.8 % of the total cation and NH4 + (mean: 164 ng m?3), accounting for 13.8 % of the total cation measured in this study. The main inorganic anions were Cl? (576 ng m?3, 54.1 %) and SO4 2? (596 ng m?3, 38.0 %). The main organic anion was oxalate (18 ng m?3). Crustal enrichment factor calculations identified 62 % of the trace elements measured (Cu, Ni, V, Co, Al, Mn, Fe, Sc, and Cr) with crustal origin. Single particle analysis demonstrated that 40 % of the aerosol particles examined were Cl? rich particles as sodium chloride from seawater and 34 % of the total particles were Si-rich particles, mainly in the form of aluminosilicates from dust material. Based on the combination of air-mass trajectories, cluster analysis and principal component analysis, the major sources of these PM2.5 particles include marine, Saharan dust and biomass burning from West Africa; however, volcanic emissions from the Soufriere Hills in Montserrat had significant impact on aerosol composition in this region at the time of sample collection.  相似文献   

17.
A box model is used to explore the detailed chemistry of C2 and C3 organic compounds in the marine troposphere by tracing the individual reaction paths resulting from the oxidation of ethane, ethene, acetylene, propane, propene and acetic acid. The mechanisms include chemical reactions in the gas phase and in the aqueous phase of clouds and aerosol particles at cloud level under conditions resembling those in the northern hemisphere. Organic hydroperoxides are found to be important intermediate products, with subsequent reactions leading partly to the formation of mixed hydroxy or carbonyl hydroperoxides that are readily absorbed into cloud water, where they contribute significantly to the formation of multifunctional organic compounds and organic acids. Organic hydroperoxides add little to the oxidation of sulfur dioxide dissolved in the aqueous phase, which is dominated by H2O2. Next to acetaldehyde and acetone, glycol aldehyde, glyoxal, methyl glyoxal and hydroxy propanone are prominent oxidation products in the gas and the aqueous phase. Acetaldehyde is not efficiently converted to acetic acid in clouds; the major local sources of acetic acid are gas-phase reactions. Other acids produced include hydroperoxy acetic, glycolic, glyoxylic, oxalic, pyruvic, and lactic acid. The mechanism of Schuchmann et al. (1985), which derives glycolic and glyoxylic acid from the oxidation of acetate, is found unimportant in the marine atmosphere. The principal precursors of glyoxylic acid are glyoxal and glycolic acid. The former derives mainly from acetylene and ethene, the latter from glycolaldehyde, also an oxidation product of ethene. The oxidation of glyoxylic acid leads to oxalic acid, which accumulates and is predicted to reach steady state concentrations in the range 30–90 ng m−3. This is greater, yet of the same magnitude, than the concentrations observed over the remote Pacific Ocean.  相似文献   

18.
An experimental study of the scavenging of dichloromethane vapor by water drops falling at terminal velocity, has been carried out in the UCLA precipitation shaft, in order to test the predictions of theoretical washout models. Whereas good agreement between theory and experiment was found for drops of radius 0.332 mm, computed gas uptake rates for 1.253 and 2.21 mm radius drops were much slower than those measured, just as reported previously for the washout of both sulfur dioxide and acetaldehyde. An analysis shows that theory can be reconciled with all of the experimental data by replacing the compound specific aqueous phase Fickian molecular diffusion coefficient used in the theory, by an effective diffusivity, having a constant value, (3×10-4 cm2 s-1), independent of the physical and chemical nature of the absorbed species, for all drops of equivalent radii greater than 0.9 mm.  相似文献   

19.
The concentrations of PM10, PM2.5 and their water-soluble ionic species were determined for the samples collected during January to December, 2007 at New Delhi (28.63° N, 77.18° E), India. The annual mean PM10 and PM2.5 concentrations (± standard deviation) were about 219 (± 84) and 97 (±56) μgm−3 respectively, about twice the prescribed Indian National Ambient Air Quality Standards values. The monthly average ratio of PM2.5/PM10 varied between 0.18 (June) and 0.86 (February) with an annual mean of ∼0.48 (±0.2), suggesting the dominance of coarser in summer and fine size particles in winter. The difference between the concentrations of PM10 and PM2.5, is deemed as the contribution of the coarse fraction (PM10−2.5). The analyzed coarse fractions mainly composed of secondary inorganic aerosols species (16.0 μgm−3, 13.07%), mineral matter (12.32 μgm−3, 10.06%) and salt particles (4.92 μgm−3, 4.02%). PM2.5 are mainly made up of undetermined fractions (39.46 μgm−3, 40.9%), secondary inorganic aerosols (26.15 μgm−3, 27.1%), salt aerosols (22.48 μgm−3, 23.3%) and mineral matter (8.41 μgm−3, 8.7%). The black carbon aerosols concentrations measured at a nearby (∼300 m) location to aerosol sampling site, registered an annual mean of ∼14 (±12) μgm−3, which is significantly large compared to those observed at other locations in India. The source identifications are made for the ionic species in PM10 and PM2.5. The results are discussed by way of correlations and factor analyses. The significant correlations of Cl−, SO42−, K+, Na+, Ca2+, NO3− and Mg2+ with PM2.5 on one hand and Mg2+ with PM10 on the other suggest the dominance of anthropogenic and soil origin aerosols in Delhi.  相似文献   

20.
The new European Council Directive (PE-CONS 3696/07) frames the inhalable (PM10) and fine particles (PM2.5) on priority to chemically characterize these fractions in order to understand their possible relation with health effects. Considering this, PM2.5 was collected during four different seasons to evaluate the relative abundance of bulk elements (Cl, S, Si, Al, Br, Cu, Fe, Ti, Ca, K, Pb, Zn, Ni, Mn, Cr and V) and water soluble ions (F−, Cl−, NO2 −, NO3 −, SO4 2−, Na+, NH4 +, Ca2+ and Mg2+) over Menen, a Belgian city near the French border. The air quality over Menen is influenced by industrialized regions on both sides of the border. The most abundant ionic species were NO3 −, SO4 2− and NH4 +, and they showed distinct seasonal variation. The elevated levels of NO3 − during spring and summer were found to be related to the larger availability of the NOx precursor. The various elemental species analyzed were distinguished into crustal and anthropogenic source categories. The dominating elements were S and Cl in the PM2.5 particles. The anthropogenic fraction (e.g. Zn, Pb, and Cu) shows a more scattered abundance. Furthermore, the ions and elemental data were also processed using principal component analysis and cluster analysis to identify their sources and chemistry. These approach identifies anthropogenic (traffic and industrial) emissions as a major source for fine particles. The variations in the natural/anthropogenic fractions of PM2.5 were also found to be a function of meteorological conditions as well as of long-range transport of air masses from the industrialized regions of the continent. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

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