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1.
Using the chemical composition of snow and ice of a central Greenland ice core, we have investigated changes in atmospheric HNO3 chemistry following the large volcanic eruptions of Laki (1783), Tambora (1815) and Katmai (1912). The concentration of several cations and anions, including SO 4 2– and NO 3 – , were measured using ion chromatography. We found that following those eruptions, the ratio of the concentration of NO 3 – deposited during winter to that deposited during summer was significantly higher than during nonvolcanic periods. Although we cannot rule out that this pattern originates from snow pack effects, we propose that increased concentrations of volcanic H2SO4 particles in the stratosphere may have favored condensation and removal of HNO3 from the stratosphere during Arctic winter. In addition, this pattern might have been enhanced by slower formation of HNO3 during summer, caused by direct consumption of OH through oxidation of volcanic SO2.  相似文献   

2.
A one-dimensional model of polar stratospheric cloud (PSC) formation and evolution during the polar winter, incorporating both HNO3 and H2O condensation, has been developed to investigate the interactions between Type I and Type II PSCs and the effects of these clouds on the stratospheric composition. Model simulations for various meteorological conditions and the results of extensive sensitivity tests are presented. Temperature oscillations, which have been included in the model, are shown to have an important influence on the characteristics and effects of the PSCs. The predicted proportions of the PSCs are consistent with observations of number, size, and optical effects, such as depolarization. Denitrification of stratospheric air by 35–88% is shown to occur in the presence of both Type I and Type II PSCs, with comparable nitrate removal in both types of clouds. Dehydration by Type II clouds simultaneously removes similar percentages of water vapour, up to 79% at lower altitudes. Altough dehydration is insensitive to most of the parameter variations except the minimum temperature, the process of denitrification, especially the proportion removed by Type I PSCs, is highly variable.  相似文献   

3.
The photodissociation coefficient of NO2, J NO 2, has been measured from a balloon platform in the stratosphere. Results from two balloon flights are reported. High Sun values of J NO 2 measured were 10.5±0.3 and 10.3±0.3×10-3 s-1 at 24 and 32 km respectively. The decrease in J NO 2 at sunset was monitored in both flights. The measurements are found to be in good agreement with calculations of J NO 2 using a simplified isotropic multiple scattering computer routine.  相似文献   

4.
A global three-dimensional model of the tropospheric sulfur cycle   总被引：9，自引：0，他引：9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

5.
Coupled the photosynthesis with transpiration and adjustment of stoma,a dynamic ecological model for simulating the canopy photosynthesis of winter wheat was established by scaling up from the biochemical scale to canopy scale,in which the effects of O3,CO2 and solar spectrum on crop photosynthesis were fully considered.Validation of the model against the data measured with CI-301PS portable photosynthesis analyzer showed that the leaf photosynthesis model passed the correlation significance test and had a fairly high accuracy.Numerical analysis showed that the canopy photosynthesis rate would be reduced by 29% if the O3 concentration increases from 0 ppbv to 200 ppbv,whereas the canopy photosynthesis rate would increase by about 37% while the CO2 concentration increases from 330 ppmv to 660 ppmv,and the canopy photosynthesis rate would be reduced by 27%0 or so under the condition that the spectrum coefficient changed from 0.5 to 0.4.If the O3 concentration reached 200 ppbv at noon on the typical sunny day with higher radiation,the canopy photosynthesis will be reduced slightly in the suburb area where the pollution is serious and the photochemical fog is easy to be formed,contrast with that in the clear region and regardless of the climate change,due to the fact that the positive effect of CO2 on crop photosynthesis can not compensate the negative effect of O3 on crop photosynthesis.The canopy photosynthesis will be reduced by 35% or so than the BASE value at present,when the spectrum of photosynthetic active radiation(PAR) reduces to 0.4 or so.  相似文献   

6.
A global ocean general circulation model (L30T63) is employed to study the uptake and distribution of anthropogenic CO2 in the ocean. A subgrid-scale mixing scheme called GM90 is used in the model. There are two main GM90 parameters including isopycnal diffusivity and skew (thickness) diffusivity. Sensitivities of the ocean circulation and the redistribution of dissolved anthropogenic CO2 to these two parameters are examined. Two runs estimate the global oceanic anthropogenic CO2 uptake to be 1.64 and 1.73 Pg C yr-1 for the 1990s, and that the global ocean contained 86.8 and 92.7 Pg C of anthropogenic CO2 at the end of 1994, respectively. Both the total inventory and uptake from our model are smaller than the data-based estimates. In this presentation, the vertical distributions of anthropogenic CO2 at three meridional sections are discussed and compared with the available data-based estimates. The inventory in the individual basins is also calculated. Use of large isopycnal diffusivity can generally improve the simulated results, including the exchange flux, the vertical distribution patterns, inventory, storage, etc. In terms of comparison of the vertical distributions and column inventory, we find that the total inventory in the Pacific Ocean obtained from our model is in good agreement with the data-based estimate, but a large difference exists in the Atlantic Ocean, particularly in the South Atlantic. The main reasons are weak vertical mixing and that our model generates small exchange fluxes of anthropogenic CO2 in the Southern Ocean. Improvement in the simulation of the vertical transport and sea ice in the Southern Ocean is important in future work.  相似文献   

7.
Two cases of simultaneous nighttime measurements of NO2 and OClO in the winter polar stratosphere are analyzed in order to test our present knowledge of halogen chemistry in the presence of high amount of NO2 at low temperature. Comparisons with Lagrangian model calculations using several hypotheses are performed. First simulations, using the admitted constant rates of chemical reaction, strongly underestimate the measured OClO while the NO2 profiles are correctly reproduced. If uncertainties in actinic fluxes calculations are taken into account, simulation results do not show a significant reduction of the underestimation. A better agreement can be achieved if the formation of unstable isomers of ClONO2 and of BrONO2 occurs in the cold conditions of the polar stratosphere. An approximate value of the branching ratios of the channels leading to ClONO2 and ClOONO, and to BrONO2 and BrOONO, necessary to reproduce both OClO and NO2 is given and discussed.  相似文献   

8.
The growth of monodisperse particles (0.07 to 0.5 µm) exposed to SO2 (0–860 ppb), H2O2 (0–150 ppb) and sometimes NH3 (0–550 ppb) in purified air at 22 °C at relative humidities ranging from 25 to 75% were measured using the Tandem Differential Mobility Analyzer technique. The experiments were performed in a flow reactor with aqueous (NH4)2SO4 and Na2SO4 droplets. For (NH4)2SO4 droplets the fractional diameter growth was independent of size above 0.3 µm but decreased with decreasing size below that. When NH3 was added the fractional growth increased with decreasing size. Measurements were compared with predictions of a model that accounts for solubility of the reactive gases, the liquid phase oxidation of SO2 by H2O2, and ionic equilibria. Agreement between measured and predicted droplet growth is reasonable when the ionic strength effects are included. Theory and experiments suggest that NH3 evaporation is responsible for the decrease in relative growth rates for small aqueous ammonium sulfate particles. The observed droplet growth rates are too slow to explain observed growth rates of secondary atmospheric sulfate particles.  相似文献   

9.
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10.
Simultaneous measurements of peroxy and nitrate radicals at Schauinsland   总被引：3，自引：0，他引：3  
We present simultaneous field measurements of NO3 and peroxy radicals made at night in a forested area (Schauinsland, Black Forest, 48° N, 8° N, 1150 ASL), together with measurements of CO, O3, NO x , NO y , and hydrocarbons, as well as meteorological parameters. NO2, NO3, HO2, and (RO2) radicals are detected with matrix isolation/electron spin resonance (MIESR). NO3 and HO2 were found to be present in the range of 0–10 ppt, whilst organic peroxy radicals reached concentrations of 40 ppt. NO3, RO2, and HO2 exhibited strong variations, in contrast to the almost constant values of the longer lived trace gases. The data suggest anticorrelation between NO3 and RO2 radical concentrations at night.The measured trace gas set allows the calculation of NO3 and peroxy radical concentrations, using a chemical box model. From these simulations, it is concluded that the observed anthropogenic hydrocarbons are not sufficient to explain the observed RO2 concentrations. The chemical budget of both NO3 and RO2 radicals can be understood if emissions of monoterpenes are included. The measured HO2 can only be explained by the model, when NO concentrations at night of around 5 ppt are assumed to be present. The presence of HO2 radicals implies the presence of hydroxyl radicals at night in concentrations of up to 105 cm–3.  相似文献   

11.
Series of high-resolution infrared solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, between 06/1986 and 11/1992, and at Kitt Peak National Observatory, Tucson, Arizona (U.S.A.), from 12/1980 to 04/1992, have been analyzed to provide a comprehensive ensemble of vertical column abundances of CHCIF2 (HCFC-22; Freon-22) above the European and the North American continents. The columns were derived from nonlinear least-squares curve fittings between synthetic spectra and the observations containing the unresolved 2v 6 Q-branch absorption of CHCIF2 at 829.05 cm–1. The changes versus time observed in these columns were modeled assuming both an exponential and a linear increase with time. The exponential rates of increase at one-sigma uncertainties were found equal to (7.0±0.35)%/yr for the Junfraujoch data and (7.0±0.23)%/yr for the Kitt Peak data. The exponential trend of 7.0%/yr found at both stations widely separated in location can be considered as representative of the global increase of the CHCIF2 burden in the Earth's atmosphere during the period 1980 to 1992. When assuming two realistic vertical volume mixing ratio profiles for CHCIF2 in the troposphere, one quasi constant and the other decreasing by about 13% from the ground to the tropopause, the concentrations for mid-1990 were found to lie between 97 and 111 pptv (parts per trillion by volume) at the 3.58 km altitude of the Jungfraujoch and between 97 and 103 pptv at Kitt Peak, 2.09 km above sea level. Corresponding values derived from calculations using a high vertical resolution-2D model and recently compiled HCFC-22 releases to the atmosphere, were equal to 107 and 105 pptv, respectively, in excellent agreement with the measurements. The model calculated lifetime of CHCIF2 was found equal to 15.6 years. The present results are compared critically with similar data found in the literature. On average, the concentrations found here are lower by 15–20% than those derived from in situ investigations; this difference cannot be explained by the absolute uncertainty of ±11% assigned presently to the infrared remote measurements.  相似文献   

12.
在膜基—气体吸收耦合实验装置上,评价了疏水性PP(聚丙烯)微孔膜,活化MDEA(N-甲基二乙醇胺)溶液分离混合气中CO2传质性能,研究了气液流速、吸收剂和混合气的浓度等因素对总传质系数的影响,采用阻力层关联方程模型预测总传质系数Kov值。结果表明:活化MDEA溶液能提高总传质系数Kov值,模型的计算值和实验值符合较好。  相似文献   

13.
The objective of this study was to reconstruct light extinction coefficients (b ext ) according to chemical composition components of particulate matter up to 2.5 μm in size (PM 2.5 ). PM 2.5 samples were collected at the monitoring station of the South China of Institute of Environmental Science (SCIES, Guangzhou, China) during January 2010, and the online absorbing and scattering coefficients were obtained using an aethalometer and a nephelometer. The measured values of light absorption coefficient by particle (b ap ) and light scattering coefficient by particle (b sp ) significantly correlated (R 2 > 0.95) with values of b ap and b sp that were reconstructed using the Interagency Monitoring of Protected Visual Environments (IMPROVE) formula when RH was <70%. The measured b ext had a good correlation (R 2 > 0.83) with the calculated b ext under ambient RH conditions. The result of source apportionment of b ext showed that ammonium sulfate [(NH 4 ) 2 SO 4 ] was the largest contributor (35.0%) to b ext , followed by ammonium nitrate (NH 4 NO 3 , 22.9%), organic matter (16.1%), elemental carbon (11.8%), sea salt (4.7%), and nitrogen dioxide (NO 2 , 9.6%). To improve visibility in Guangzhou, the effective control of secondary particles like sulfates, nitrates, and ammonia should be given more attention in urban environmental management.  相似文献   

14.
采用基于离子液体[Bmin][BF4]+AMP作为捕集CO2的复合溶液,在膜吸收-热再生循环装置上,研究了该复合溶液捕集CO2的过程和传质性能;通过阻力层传质模型,比较了预测值与实验值.结果表明：在相同条件和较高负载下,复合溶液具有较高的传递推动力和更高的传质系数;模型预测值和实验值符合较好,平均误差为12.8%.实验证明复合溶液的传质性能优于单一溶液.  相似文献   

15.
A basin-wide ocean general circulation model(OGCM) of the Pacific Ocean is employed to estimate the uptake and storage of anthropogenic CO 2 using two different simulation approaches.The simulation(named BIO) makes use of a carbon model with biological processes and full thermodynamic equations to calculate surface water partial pressure of CO 2,whereas the other simulation(named PTB) makes use of a perturbation approach to calculate surface water partial pressure of anthropogenic CO 2.The results from the two simulations agree well with the estimates based on observation data in most important aspects of the vertical distribution as well as the total inventory of anthropogenic carbon.The storage of anthropogenic carbon from BIO is closer to the observation-based estimate than that from PTB.The Revelle factor in 1994 obtained in BIO is generally larger than that obtained in PTB in the whole Pacific,except for the subtropical South Pacific.This,to large extent,leads to the difference in the surface anthropogenic CO 2 concentration between the two runs.The relative difference in the annual uptake between the two runs is almost constant during the integration processes after 1850.This is probably not caused by dissolved inorganic carbon(DIC),but rather by a factor independent of time.In both runs,the rate of change in anthropogenic CO 2 fluxes with time is consistent with the rate of change in the growth rate of atmospheric partial pressure of CO 2.  相似文献   

16.
An observational campaign was conducted in the street canyon of Zhujiang Road in Nanjing city in 2007.Hourly mean concentrations of PM10 were measured at street and roof levels.The Operational Street Pollution Model(OSPM)street canyon dispersion model was used to calculate the street concentrations and the results were compared with the measurements.The results show that there is good agreement between measured and predicted concentrations.The correlation coecient R2 values(R2 is a measure of the correlation of the predicted and measured time series of concentrations)are 0.5319,0.8044,and 0.6630 for the scatter plots of PM10 corresponding to light wind speed conditions,higher wind speed conditions,and all wind speed conditions,respectively.PM10 concentrations tend to be smaller for the higher wind speed cases and decrease rapidly with increasing wind speed.The presentations of measured and modelled concentration dependence on wind direction show fairly good agreement.PM10 concentrations measured on the windward side are relatively smaller,compared with the corresponding results for the leeward side.This study demonstrates that it is possible to use the OSPM to model PM10 dispersion rules for an urban street canyon.  相似文献   

17.
The limited area model MAR (Modèle Atmosphérique Régional) is validated over the Antarctic Plateau for the period 2004–2006, focussing on Dome C during the cold season. MAR simulations are made by initializing the model once and by forcing it through its lateral and top boundaries by the ECMWF operational analyses. Model outputs compare favourably with observations from automatic weather station (AWS), radiometers and atmospheric soundings. MAR is able to simulate the succession of cold and warm events which occur at Dome C during winter. Larger longwave downwelling fluxes (LWD) are responsible for higher surface air temperatures and weaker surface inversions during winter. Warm events are better simulated when the small Antarctic precipitating snow particles are taken into account in radiative transfer computations. MAR stratosphere cools during the cold season, with the coldest temperatures occurring in conjunction with warm events at the surface. The decrease of saturation specific humidity associated with these coldest temperatures is responsible for the formation of polar stratospheric clouds (PSCs) especially in August-September. PSCs then contribute to the surface warming by increasing the surface downwelling longwave flux.  相似文献   

18.
一次降雹过程的AgI系列催化模拟研究   总被引：1，自引：1，他引：0       下载免费PDF全文
云数值模拟是研究降雹过程和人工防雹试验的重要手段。利用三维冰雹云AgI催化模式,对北京1996年6月10日的一次降雹过程进行AgI不同催化高度、催化剂量和催化时间的系列催化模拟试验,并优选催化方案,为外场防雹设计和作业提供依据。在催化系列模拟中发现,不同催化高度的催化剂均在上升到-5℃高度后开始核化。在2.1~4.9 km高度范围内催化,AgI成核率比较高,防雹效果较好。核化的人工冰晶有效弥补了该高度上自然冰晶的不足。小剂量催化,可在减雹的同时增加部分降雨量,而大剂量催化,在减雹的同时会减少降雨。在催化时间、剂量和高度的系列催化试验中得出,采用在模拟的第15分钟在5 km高度附近播撒AgI,连续4次以5×106 kg-1的催化剂量进行催化,催化效果较好,可减少降雹量约60%,同时可避免降雨量的大幅减少。  相似文献   

19.
During the 1982 and 1983 Balloon Intercomparison Campaigns, the vertical profile of stratospheric NO2 was measured remotely by nine instruments and that of NO by two. Total overhead columns were measured by two more instruments. Between 30 and 35km, where measurements overlapped, agreement between NO profiles was within ±30%, which is better than the accuracies claimed by the experimenters. Between 35 and 40km there was similarly good agreement between NO2 profiles, but below 30km, differences of greater than a factor three were found. In the second Campaign, NO2 values from most instruments agreed within their quoted errors, except that the Oxford radiometer gave much lower values; but the first Campaign and the column measurements show a more uniform spread of results.These differences below 30km could not be resolved, but new laboratory measurements are planned which should do so.  相似文献   

20.
We present mobile vehicle lidar observations in Tianjin, China during the spring, summer, and winter of 2016. Mobile observations were carried out along the city border road of Tianjin to obtain the vertical distribution characteristics of PM2.5. Hygroscopic growth was not considered since relative humidity was less than 60% during the observation experiments. PM2.5 profile was obtained with the linear regression equation between the particle extinction coefficient and PM2.5 mass concentration. In spring, the vertical distribution of PM2.5 exhibited a hierarchical structure. In addition to a layer of particles that gathered near the ground, a portion of particles floated at 0.6–2.5-km height. In summer and winter, the fine particles basically gathered below 1 km near the ground. In spring and summer, the concentration of fine particles in the south was higher than that in the north because of the influence of south wind. In winter, the distribution of fine particles was opposite to that measured during spring and summer. High concentrations of PM2.5 were observed in the rural areas of North Tianjin with a maximum of 350 μg m–3 on 13 December 2016. It is shown that industrial and ship emissions in spring and summer and coal combustion in winter were the major sources of fine particles that polluted Tianjin. The results provide insights into the mechanisms of haze formation and the effects of meteorological conditions during haze–fog pollution episodes in the Tianjin area.  相似文献   

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