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《Atmospheric Environment. Part A. General Topics》1992,26(3):465-484
Acid deposition in the eastern U.S. during a spring frontal storm from 1 to 5 May 1985 is analysed using the STEM-II acid deposition model. Nitrate formation is dominated by gas-phase production processes, with wet and dry deposition contributing equally to the total domain nitrate deposition. In-cloud sulfate production accounts for 60% of the total sulfate production, while wet deposition dominates the total sulfate deposition. Oxidation of S(IV) by hydrogen peroxide is the most important sulfate formation pathway. Hydrogen peroxide is found to exist in excess of S(IV) in cloud and rainwater in the storm front and at altitudes above 2 km. Production rates of sulfate in the high sulfur source regions are significantly lower (up to an order of magnitude) than in the moderate or low source regions. Model predictions are shown to capture the major features of the observed deposition. 相似文献
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《Atmospheric Environment. Part A. General Topics》1991,25(8):1577-1590
Diurnal curves of tropospheric ozone are characterized for the areas near coniferous forests in the western U.S. A given day of hourly data can be placed into one of 17 classes of diurnal curves simply by knowing the 24-h mean and coefficient of variation of range, or more precisely, by applying equations derived from our discriminant analysis. The variation among curves is known to be related to theory of ozone formation, scavenging, and transport. Season, latitude, and position relative to source areas affect the form of the diurnal curve. 相似文献
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《Atmospheric Environment. Part A. General Topics》1990,24(2):415-421
Concentrations of Mn from soil dust and anthropogenic emissions were studied in the aerosols collected at Mayville, NY. The southwest quadrant of this rural site has numerous Mn-emitting sources. Aerosols arriving from this quadrant contained 80–90% Mn of anthropogenic origin, the remainder was soil derived. Bivariate analysis showed a good linear correlation between noncrustal Mn and Fe, indicating that anthropogenic Mn was mainly derived from the iron and steel industry. Aerosols with relatively high Mn concentrations and enrichments were also encountered during the study period. These were attributed to nonferrous industries such as silico-manganese alloy, synthetic pyrolusite and Mn chemical manufacturing plants. Comparison of concentrations, enrichment factors and ratios of the two elements, Mn and Fe, in these aerosols and in aerosols from several midwestern cities located in the vicinity of Mn-emitting sources attested to the inferences drawn above. Several Mn-emitting sources in the States of Ohio and Pennsylvania were shown to be causative for the high noncrustal Mn concentration at Mayville relative to those seen in rural aerosols from Ashland County, OH, and Shenandoah Valley, VA as well as for the relatively high ratio of noncrustal Mn/Se reported for the lower midwest signature in our earlier study. 相似文献
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平流层臭氧在特定气象条件下可侵入对流层,严重情况下会引发近地面监测点位的臭氧浓度超标。美国环境保护局(EPA)将上述事件称作"平流层臭氧侵入例外事件"(以下简称"例外事件"),并于2018年颁布了《关于可能影响臭氧浓度的平流层臭氧侵入例外事件申请陈述指南》(以下简称《指南》)。本文结合美国相关实操案例,详细阐述了"例外事件"的识别、判定技术和业务化处理流程及其对我国探索开展"例外事件"剔除工作的启示,以期为我国臭氧污染管控提供决策参考。研究发现以下结果:一是"例外事件"不定期发生,且影响范围较大,直接导致受影响区域近地面监测点位臭氧浓度异常超标,影响臭氧达标限值的设定,不利于客观公平地开展空气质量达标考核工作;二是美国依托多种监测手段和模式方法,已针对"例外事件"形成了一套完整的判定指标体系及规范的业务化流程,可直接扣除此类事件导致的臭氧超标数据;三是美国现有实操案例多为解决平流层臭氧侵入导致西部高海拔地区(如怀俄明州、犹他州等)近地面臭氧浓度超标的问题。地方空气质量管理机构只有在"例外事件"发生期间臭氧浓度处于年度排名前四位时,才会积极组织相关技术专家开展"例外事件"的证据搜集和申请工作。"例外事件"美国做法对我国的启示是:尽快组织力量深入开展我国"例外事件"的回溯分析,重点关注春末和冬初以臭氧为首要污染物的轻度污染天气,尽快形成我国"例外事件"的识别判定技术规范与要求,并建立健全"例外事件"管理机制,为打赢污染防治攻坚战提供有力支撑。 相似文献
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《Atmospheric Environment. Part A. General Topics》1991,25(2):305-315
From 1975 to 1987 a 19% change in SO2 emissions a 16% change in NOx emissions have occurred over the eastern and mid-western U.S. Six continental precipitation chemistry sites from the MAP3S network, plus the Hubbard Brook Experimental Forest, NH, show a direct relationship between emission levels and precipitation H+ and SO42- concentrations, except for Penn State, PA. MAP3S sites at Illinois and Ohio, located closest to the major SO2 source regions, demonstrates statiscally significant (P <0.05) linear regressions of SO42- concentrations on SO2 emissions. Whiteface Mt., NY, shows a weaker relationship (P <0.01), and Hubbard Brook shows the strongest relationship (P <0.01) between SO2 emissions and SO42- concentration in precipitation. No site shows a significant relationship (P <0.10) for NOx emissions and NO3− concentrations in precipitation. Illinois, Ohio, Ithaca and Hubbard Brook show significant linear regressions of H+ concentrations on emissions of SO2 + NOx (P <0.10, 0.05, 0.01, and 0.01, respectively). Overall, for the entire region examined, decreasing SO2 emissions levels appear to have decreased SO42- concentrations with an efficiency of 74% ± 15% (s.e.). Decreasing SO2 plus NOx emissions (18%) have been accompanied by a decreasing H+ concentrations (18%) suggesting an efficiency of conversion of 100% ± 15% (s.e.) for the study region as a whole. While significant reductions in acid species have occured at Hubbard Brook, further reductions in excess of 50% of present deposition are necessary to protect acid-sensitive ecosystems. 相似文献
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《Environmental Science & Policy》1999,2(4-5):397-411
The 188 air contaminants designated as hazardous air pollutants, or air toxics, under the Clean Air Act Amendments of 1990 are associated with a variety of adverse human health impacts. The US Environmental Protection Agency recently developed estimates of 1990 outdoor concentrations of 148 air toxics for every census tract in the continental United States. This paper compares the results for urban and rural areas, and evaluates the relative contributions of large stationary sources (point sources), small stationary sources (area sources), and mobile sources. The estimated air toxics concentrations in urban areas were typically twice as high as in rural areas. There were more air toxics with modeled ambient concentrations in excess of health benchmarks in urban census tracts than in rural census tracts. Ambient concentrations attributable to area sources alone exceeded health benchmarks in a majority of urban census tracts for several pollutants; similar results were found for mobile sources. For point sources, exceedances of benchmarks generally occurred in fewer census tracts. These results show that reductions in emissions of air toxics from all three types of sources will be necessary to reduce anthropogenic air toxics concentrations to levels below the health benchmark concentrations. 相似文献
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Jia Mao Lili Wang Chuhan Lu Jingda Liu Mingge Li Guiqian Tang Dongsheng Ji Nan Zhang Yuesi Wang 《环境科学学报(英文版)》2020,32(6):187-199
An intensive and persistent regional ozone pollution event occurred over eastern China from 25 June to 5 July 2017.73 out of 96 selected cities,most located in the Beijing-TianjinHebei and the surrounding area(BTHS),suffered severe ozone pollution.A north-south contrast ozone distribution,with higher ozone(199±33 μg/m3) in the BTHS and lower ozone(118±25 μg/m3) in the Yangtze River Delta(YRD),was found to be dominated by the position of the West Pacific Subtropical High(WPS... 相似文献
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《Advances in Environmental Research》2004,8(1):137-146
Arsenic contamination is of great environmental concern due to its toxic effects as a carcinogen. Knowledge of arsenic background concentrations is important for land application of wastes and for making remediation decisions. The soil clean-up target level for arsenic in Florida (0.8 and 3.7 mg kg−1 for residential and commercial areas, respectively) lies within the range of both background and analytical quantification limits. The objective of this study was to compare arsenic distribution in urban and non-urban areas of Florida. Approximately 440 urban and 448 non-urban Florida soil samples were compared. For urban areas, soil samples were collected from three land-use classes (residential, commercial and public land) in two cities, Gainesville and Miami. For the non-urban areas, samples were collected from relatively undisturbed non-inhabited areas. Arsenic concentrations varied greatly in Gainesville, ranging from 0.21 to approximately 660 mg kg−1 with a geometric mean (GM) of 0.40 mg kg−1, which were lower than Miami samples (ranging from 0.32 to 112 mg kg−1; GM=2.81 mg kg−1). Arsenic background concentrations in urban soils were significantly greater and showed greater variation than those from relatively undisturbed non-urban soils (GM=0.27 mg kg−1) in general. 相似文献
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Tait Chirenje Lena Q. MaMing Chen Edward J. Zillioux 《Advances in Environmental Research》2003,8(1):137-146
Arsenic contamination is of great environmental concern due to its toxic effects as a carcinogen. Knowledge of arsenic background concentrations is important for land application of wastes and for making remediation decisions. The soil clean-up target level for arsenic in Florida (0.8 and 3.7 mg kg−1 for residential and commercial areas, respectively) lies within the range of both background and analytical quantification limits. The objective of this study was to compare arsenic distribution in urban and non-urban areas of Florida. Approximately 440 urban and 448 non-urban Florida soil samples were compared. For urban areas, soil samples were collected from three land-use classes (residential, commercial and public land) in two cities, Gainesville and Miami. For the non-urban areas, samples were collected from relatively undisturbed non-inhabited areas. Arsenic concentrations varied greatly in Gainesville, ranging from 0.21 to approximately 660 mg kg−1 with a geometric mean (GM) of 0.40 mg kg−1, which were lower than Miami samples (ranging from 0.32 to 112 mg kg−1; GM=2.81 mg kg−1). Arsenic background concentrations in urban soils were significantly greater and showed greater variation than those from relatively undisturbed non-urban soils (GM=0.27 mg kg−1) in general. 相似文献
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Most previous O3 simulations were based only on gaseous phase photochemistry. However, some aerosol-related processes, namely, heterogeneous reactions occurring on the aerosol surface and photolysis rate alternated by aerosol radiative influence, may affect O3 photochemistry under high aerosol loads. A three-dimensional air quality model, Models-3/Community Multi-scale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution, was employed to simulate the effects of the above-mentioned processes on O3 formation under typical high O3 episodes in Beijing during summer. Five heterogeneous reactions, i.e., NO2, NO3, N2O5, HO2, and O3, were individually investigated to elucidate their effects on O3 formation. The results showed that the heterogeneous reactions significantly affected O3 formation in the urban plume. NO2 heterogeneous reaction increased O3 to 90 ppb, while HO2 heterogeneous reaction decreased O3 to 33 ppb. In addition, O3 heterogeneous loss decreased O3 to 31 ppb. The effects of NO2, NO3, and N2O5 heterogeneous reactions showed opposite O3 concentration changes between the urban and extra-urban areas because of the response of the reactions to the two types of O3 formation regimes. When the aerosol radiative influence was included, the photolysis rate decreased and O3 decreased significantly to 73 ppb O3. The two aerosol-related processes should be considered in the study of O3 formation because high aerosol concentration is a ubiquitous phenomenon that affects the urban- and regional air quality in China. 相似文献
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《Atmospheric Environment. Part A. General Topics》1993,27(6):845-865
The long-range transport of air pollutants (LRTAP) over Europe is studied by a mathematical model based on a system of partial differential equations (PDEs). The number of PDEs is equal to the number of species studied and the model contains 35 species at present. Among the species are NO, NO2, NO3−, HNO3, NH3, NH4+, O3, PAN, SO2, SO42− and may hydrocarbons. Most of the 70 chemical reactions involved in the model are nonlinear (including here many photochemical reactions).The model requires large sets of input data. Emissions of SO2, NOx, NH3 and both natural and anthropogenic volatile organic compounds (VOC) are needed in the model. The meteorological data consist of fields of wind velocities, precipitation, surface temperatures, temperatures of the boundary layer, relative humidities and cloud cover, which are read in the beginning of every 6-h interval. Both daytime and nighttime mixing heights are used in the model.Many of the species in the model vary on a diurnal basis. An investigation of the main mechanisms that determine the diurnal variation of the ozone concentrations is performed. One of the important conditions that is necessary if one wants to represent correctly the diurnal variations of the concentrations is to have access to meteorological data that vary diurnally. This is especially true for the temperature and the mixing height.The use of modern numerical algorithms (which are combined with vectorization of the most time-consuming numerical procedures) allows one to perform long-term runs with the model on several high-speed computers. Results obtained in runs with meteorological data for July 1985 and August–October 1989 are discussed. The computed concentrations and depositions are compared with measurements taken at stations located in different European countries. The agreement between calculated concentrations and measurements is reasonably good.Results obtained with several scenarios, in which the NOx emission and/or the anthropogenic VOC emissions are varied, are presented. Several main conclusions are drawn by studying the results obtained during the comparisons. Some plans for future development of the models are discussed. 相似文献
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《Environmental Science & Policy》2000,3(4):189-199
Following the Council Directive 92/72/EEC on air pollution by ozone the Member States of the European Union have to inform the European Commission on ozone concentrations and exceedances of threshold values within their territory. Using the available information covering the period of 5 years (1994–1998), the data has been analysed for a possible trend in statistical parameters (50- and 98-percentiles) and number and severity of exceedances. Time series are relatively short but the data suggest that there might be a small increasing trend in the 50 percentile values. The ozone peak values, expressed as 98-percentile values or as number of exceedance days tend to decrease. However, these conclusions must be interpreted carefully as on the short time scales considered here meteorological variations and inter-annual changes may play an important role. The decrease in peak values is most likely caused by the decrease in European ozone precursor emissions since 1990; insufficient data is available to explain the increasing 50-percentile values. Possible explanations are an increase in tropospheric ozone background values caused by a world-wide increase in CH4, CO and NOx emissions or a reduced ozone titration by reduced NOx emissions on the local scale. The data submitted under the ozone directive is insufficient to provide firm conclusions on this point. 相似文献
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《Atmospheric Environment. Part A. General Topics》1990,24(1):185-193
Seasonal averaged ground level concentrations for O3 have been calculated for The Netherlands by means of a two-layer Lagrangian long-range transport (LRT) model. The model includes emissions, nonlinear atmospheric chemistry, dry deposition, exchange between boundary layer (BL) and free troposphere (FT) and fumigation between a mixed layer and an aged smog layer. Concentrations of primary and secondary pollutants in the FT are obtained from a two-dimensional global model developed by Isaksen.In the reference calculation the modelled concentrations of Ox (sum of O3 and NO2) and O3 are in fair agreement with measurements. The NOx (sum of NO and NO2) and NO2 concentrations are under-estimated by the model but there is a good temporal correlation between calculated and measured concentrations. Validation of other components involved in the chemical scheme is hardly possible due to the paucity of measured data. It can only be stated that the results presented in this paper are not in disagreement with measured or modelled data presented in the literature.In a number of sensitivity runs the influence of European anthropogenic emissions of NOx and volatile organic compounds (VOC) has been investigated. The calculations indicate that the influence of European emissions on the growing season, daytime averaged (May–September, 10–17 h) O3 concentrations in The Netherlands is small. For European reductions in the order of tens of per cents a VOC emission reduction is more effective than a NOx emission reduction in lowering the O3 concentrations. For strong reductions (about 70%) VOC and NOx are equally effective. The effects of the modelled underprediction of NOx concentrations on the production of O3 on a European scale are probably small. On a local scale the effects are more pronounced due to the NO/O3 titration (photostationary equilibrium). Therefore, an empirical correction is applied on the modelled O3 concentrations. After this correction, it is shown that daytime O3 levels during the growing season increase when European NOx emissions are reduced (2.0–7.7.% increase at 50% NOx emission reduction). A reduction in VOC emission leads to decreasing O3 levels (9% reduction for 40% VOC emission reduction, 16% reduction for 70% VOC emission reduction). For a combined reduction of both VOC and NOx slightly decreasing ground level O3 concentrations are expected. 相似文献
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《Atmospheric Environment. Part B. Urban Atmosphere》1991,25(2):165-175
Long-term trends in wintertime visibility are examined in eight mideastern U.S. cities in light of the underlying climatology. Using an array of meteorological elements known to be related to visibility, a synoptic climatological classification is developed, producing a baseline climate for each city. This approach allows for an analysis of long-term air quality trends which are unrelated climatic variations.Yearly mean visibility levels are closely related to climatic variations. Years with frequent occurrences of continental polar and arctic air masses and cold front passages exhibit high visibility, while low air quality is related to overrunning situations (a warm or stationary front to the south) and the advection of Atlantic maritime polar air. Winter air quality declined from the early 1950s to 1970, improved throughout the mid 1970s, and either remained steady or improved slightly thereafter. 相似文献