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1.
Ground-level ozone and oxidant (sum of O3 and NO2) concentrations in The Netherlands are calculated during the growing season (May–September) by means of a Lagrangian long-range transport model. Two air parcels—one representative of the mixed layer, the other representative of the polluted layer above the mixed layer (aged smog layer)—are followed along 96 h back trajectories. Long-term averaged and 98 percentile values of hourly averaged concentrations are estimated on the basis of concentrations calculated for four arrival times per day for all days in the period considered.In a number of sensitivity runs the influence of European anthropogenic NOx and VOC emissions on the oxidant concentrations in The Netherlands has been investigated. In general, the influence of European emissions on the 98-percentile values is 2–3 times as large as on the averaged concentrations. This indicates that long-term averaged concentrations more strongly depend on the concentrations in the free troposphere whereas the episodic concentrations are determined by photochemical production over Europe. VOC emission reduction is more effective in lowering episodic concentrations than NOx emission reduction. For long-term averaged concentrations, however, NOx and VOC emission reduction of 50% or more are nearly equally effective.  相似文献   

2.
Because of the recent growth in ground-level ozone and increased emission of volatile organic compounds (VOCs), VOC emission control has become a major concern in China. In response, emission caps to control VOC have been stipulated in recent policies, but few of them were constrained by the co-control target of PM2.5 and ozone, and discussed the factor that influence the emission cap formulation. Herein, we proposed a framework for quantification of VOC emission caps constrained by targets for PM2.5 and ozone via a new response surface modeling (RSM) technique, achieving 50% computational cost savings of the quantification. In the Pearl River Delta (PRD) region, the VOC emission caps constrained by air quality targets varied greatly with the NOx emission reduction level. If control measures in the surrounding areas of the PRD region were not considered, there could be two feasible strategies for VOC emission caps to meet air quality targets (160 µg/m3 for the maximum 8-hr-average 90th-percentile (MDA8-90%) ozone and 25 µg/m3 for the annual average of PM2.5): a moderate VOC emission cap with <20% NOx emission reductions or a notable VOC emission cap with >60% NOx emission reductions. If the ozone concentration target were reduced to 155 µg/m3, deep NOx emission reductions is the only feasible ozone control measure in PRD. Optimization of seasonal VOC emission caps based on the Monte Carlo simulation could allow us to gain higher ozone benefits or greater VOC emission reductions. If VOC emissions were further reduced in autumn, MDA8-90% ozone could be lowered by 0.3-1.5 µg/m3, equaling the ozone benefits of 10% VOC emission reduction measures. The method for VOC emission cap quantification and optimization proposed in this study could provide scientific guidance for coordinated control of regional PM2.5 and O3 pollution in China.  相似文献   

3.
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   

4.
利用Williams等和Guenther等的模型估计中国地区NOx和VOC的自然源排放.所得清单显示土壤NOx排放总量(以N计)为225.75 Gg;植被VOC年排放总量(以C计)为13.23 Tg,其中异戊二烯、单萜烯、其它VOC分别为7.77、1.86、3.60 Tg;排放有明显季节变化和空间变化.运用中尺度气象模式MM5以及光化学模式Calgrid研究这些排放在不同季节对对流层化学的影响.结果表明,O3、NOx、HNO3和PAN的全国平均浓度在土壤NOx排放影响下分别增加15.3%、15.7%、25.5%和6.5%;在植被VOC排放影响下改变5.6%、-4.9%、-19.3%和142.3%;在两者综合影响下增加26.1%、8.8%、4.3%和177.9%;浓度变化在夏季明显强于其它季节.自然源对中国地区光化学污染物空间分布有不同程度的影响,这种影响同区域气象条件、源排放和NMHC/NOx比值等因素有关.NOx和VOC的自然源排放对光化学特性影响显著,在光化学模拟过程中不容忽视.  相似文献   

5.
The study shows the variation of surface ozone concentrations for six selected sites between 410 and 3569 m elevation. The annual mean values in 1987 for these sites ranged from 10 to 50 ppb. Mean values of ozone as well as frequency of peak values are clearly dependent on the elevation of the site. Apart from elevation the influences of the specific location and exposure to pollutants such as NO and NO2 are considered. The ratio of the daily means of NO and NO2 is very well suited to indicate local sources. Mean diurnal concentration variations of nitric oxide and ozone on a slope show a significant influence of topography.  相似文献   

6.
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   

7.
Ozone concentrations over Europe have been calculated with the EMEP MSC-W ozone model for two extended summer periods: April–September 1985 and April–October 1989. The predicted monthly variations in both mean and elevated ozone levels are illustrated. The model is shown to compare satisfactorily with ozone data across nearly all the months studied, particularly in 1989. Modelled PAN and total airborne nitrate concentrations are also shown to compare favourably with the measurements of a Nordic measurement campaign in autumn 1989, although there is an unresolved discrepancy between the modelled and observed NO2 at these sites. In addition, the model has now been used to estimate the effects of NOx and volatile organic compound emission control on both mean and elevated ozone levels for 6 months in 1989.  相似文献   

8.
A field measurement campaign for ozone and ozone precursors(VOCs and NOx) was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface O3 pollution with the characteristics of high average daily mean and maximum concentrations(64.0 and 145.4 ppbV in no-rain days, respectively) and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.5–46.1 and 1.8–6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes(60.0% ± 4.3%), alkenes(21.1% ± 5.5%) and aromatics(18.9% ± 3.9%). Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15–0.27 and 0.42–0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.  相似文献   

9.
烟雾箱与数值模拟研究苯和乙苯的臭氧生成潜势   总被引:1,自引:0,他引:1  
贾龙  徐永福 《环境科学》2014,35(2):495-503
结合光化学烟雾箱实验与数值模拟研究了苯和乙苯在NO x存在条件下的光氧化臭氧生成潜势.重复实验表明,在乙苯-NO x反应体系中,反应物初始浓度、温度、湿度和光照强度接近的条件下,整个反应过程中臭氧的最大偏差仅为4%,证明了烟雾箱的可重复性较高.在烟雾箱实验的基础上,使用MCM(master chemical mechanism)模拟了苯和乙苯的光氧化O3生成,并将其结果与实验数据进行了比对分析.干燥(≤5%)时MCM对苯和乙苯的模拟结果与实验结果较接近,如在苯-NO x反应体系中,MCM模拟的O3峰值比实验值偏大20%;在湿度为5%~70%时,MCM模拟的乙苯光氧化O3峰值与实验值偏高约(10%~25%).用MCM模拟了太阳光照条件下苯和乙苯的臭氧生成等值线,得到在它们浓度为(10~50)×10-9,NO x在(10~100)×10-9时,苯和乙苯的6 h臭氧贡献值分别为(3.1~33)×10-9和(2.6~122)×10-9,臭氧峰值范围分别是(3.5~54)×10-9和(3.8~164)×10-9.此外,模拟得到苯和乙苯的最大增量反应活性(maximum incremental reactivity,MIR)值分别为0.25/C和0.97/C(每单位碳).该结果与Carter通过SAPRC机制得到的MIR值趋势一致.模拟得到苯和乙苯的最大臭氧反应活性(maximum ozone reactivity,MOR)分别为0.73/C和1.03/C.苯的MOR值远高于Carter使用SAPRC得到的结果,说明根据Carter得到的苯MOR会低估苯的O3潜势.  相似文献   

10.
夏季长三角地区臭氧非线性响应曲面模型的建立及应用   总被引:2,自引:0,他引:2  
2013年8月上旬,长三角地区发生了一次大范围高浓度臭氧污染事件.本研究基于WRF-CMAQ空气质量模型系统,结合长三角地区大气污染物排放清单,构建了臭氧与其前体物之间的非线性响应曲面模型(Response surface modeling,RSM).基于RSM探讨了长三角地区O_3化学的敏感性特征,分析了上海市O_3的来源并预测不同情景下O_3的变化,提出O_3污染的最优控制方案.研究结果表明,长三角地区夏季O3主控因素区域差别较大,上海环科院、杭州卧龙桥、南京玄武湖等城区点位属于VOC控制型;徐州铜山、合肥肥西、丽水青田等郊区属于NOx控制型.O_3的敏感性特征在不同浓度水平下也呈现较大差异,随着O_3浓度水平的升高,各地区NOx敏感性均有所增加.从区域来源来看,远距离传输对平日上海O_3贡献较大,占50%以上;而在O_3污染日,本地及区域贡献为72.1%,而远距离传输贡献下降至27.9%.快速预测了110组减排情景,表明在本地及区域前体物均减排70%的情况下,2013年8月上海O_3浓度能完全达标.  相似文献   

11.
黄丽华  莫创荣  徐永福  贾龙 《环境科学》2012,33(8):2551-2557
利用自制光化学烟雾箱模拟了丙烷和NOx大气光化学反应,研究了相对湿度以及丙烷与NOx初始浓度比值对臭氧生成的影响.实验表明,臭氧最大值及丙烷的臭氧生成活性最大值(IRmax)都随相对湿度的增大而减小.低相对湿度时,臭氧最大值大约出现在反应的22 h,IRmax变化范围为0.023 1~0.039 1;而高相对湿度时,臭氧最大值大约出现在反应的16 h,IRmax变化范围为0.017 2~0.032 0.在反应的20 h内,前12 h内相对湿度对丙酮的生成量影响不大,12 h后低相对湿度时丙酮生成量更大.在实验的4~20 h内,相对湿度为17%时,丙酮浓度为153×10-9~364×10-9;而相对湿度为62%时,丙酮浓度为167×10-9~302×10-9.臭氧最大值随着丙烷与NOx初始浓度比值增加而减少,在低相对湿度时线性负相关性更好.另外,还利用了MCM丙烷子机制对反应进行了数值模拟,并与实验结果进行比较,发现两者还存在较大的偏差.  相似文献   

12.
北京城区夏季O3化学生成过程   总被引:1,自引:2,他引:1  
选取2007年7月1日—8月31日中的21个晴空日,利用观测资料和光化学箱模式计算了北京城区测点的O3生成速率G(O3)和O3生成效率OPE.结果表明,21个晴空日中G(O3)日最高小时值分布在(18~82)×10-9h-1之间;在O3污染和非污染日G(O3)最高值的平均水平无显著差异,且与Ox浓度之间不存在一致的对应关系,表明O3化学生成过程不能全面解释地面O3浓度的累积,物理传输过程对测点O3实测浓度有显著作用;各个化学过程对G(O3)的贡献率对比结果显示,HO2 在 NO向NO2的转化中贡献最大;OPE值分布在2.8~5.8之间,总体水平为4.1±0.1;OPE值与NOx浓度之间为非线性关系,OPE值随NOx浓度的增加而减少,表明消减测点附近VOCs排放能有效降低O3浓度.  相似文献   

13.
The present study evaluates ground-based downward surface shortwave radiation (Rs) over the coastal region of Alicante (Southeastern Spain). Hourly measurements collected over the eleven-year period 2010-2020 are used. Two weather stations located over the region capital, Alicante, have been selected as representative of urban and suburban typologies. Two additional weather stations far from the city have been selected representing rural typologies. Rs is significantly reduced over the urban station during the morning hours within the winter season compared to the observations recorded over the suburban and rural stations, with a global mean difference of -81 and -120 W/m2 at 10 LT, respectively. However, no significant differences are obtained during the midday sun, with a global mean difference of -20 W/m2 between the urban and rural stations. With the aim of explaining these differences, the current paper investigates the relationship between Rs and different air pollutants: NOx, SO2, and fine particulate matter (PM2.5 and PM10) as well as the wind field measured at the urban and suburban stations. The results found in this work point towards a close relationship between Rs and NOx concentrations annual cycles, which are also influenced by the prevailing wind circulations observed over the study area. A global mean NOx concentration of 107 µg/m3 is observed over the urban station at 10 LT during the winter season. In contrast, these high concentrations are significantly reduced over the suburban station, with global mean value of 40 µg/m3 at 10 LT, for this period of the year.  相似文献   

14.
Meteorological conditions affect the ozone concentration near the surface. To quantify the importance of meteorological parameters for the surface ozone concentration a nonlinear regression analysis between 313 meteorological candidate predictors and surface ozone concentration at five stations in the German Democratic Republic over the period 1972–1987 has been made. The stability and quality of the relationship between ozone and meteorological predictors has been tested by independent samples. Most important predictors for surface ozone are the ozone value of the preceding day (persistence) and solar radiation. They explain 33–46% and 6–21% of the climatological ozone variance, respectively. As all meteorological parameters can be forecasted, the regression method described might be the basis for a short-term prediction of surface ozone. An analysis of long-term changes of surface ozone and solar radiation shows that changes in cloudiness are probably not the main cause of the long-term changes in surface ozone. Therefore, the ozone changes should mainly be due to changes in circulation and/or concentration of ozone precursors (NOx, VOC).  相似文献   

15.
Based on the observation by a Regional Air Quality Monitoring Network including 16 monitoring stations, temporal and spatial variations of ozone(O3), NO2and total oxidant(Ox) were analyzed by both linear regression and cluster analysis. A fast increase of regional O3concentrations of 0.86 ppbV/yr was found for the annual averaged values from 2006 to 2011 in Guangdong, China. Such fast O3increase is accompanied by a correspondingly fast NOx reduction as indicated by a fast NO2 reduction rate of 0.61 ppbV/yr. Based on a cluster analysis, the monitoring stations were classified into two major categories – rural stations(non-urban) and suburban/urban stations. The O3concentrations at rural stations were relatively conserved while those at suburban/urban stations showed a fast increase rate of 2.0 ppbV/yr accompanied by a NO2 reduction rate of 1.2 ppbV/yr. Moreover, a rapid increase of the averaged O3 concentrations in springtime(13%/yr referred to 2006 level) was observed, which may result from the increase of solar duration, reduction of precipitation in Guangdong and transport from Eastern Central China. Application of smog production algorithm showed that the photochemical O3production is mainly volatile organic compounds(VOC)-controlled. However, the photochemical O3production is sensitive to both NOx and VOC for O3pollution episode. Accordingly, it is expected that a combined NOx and VOC reduction will be helpful for the reduction of the O3 pollution episodes in Pearl River Delta while stringent VOC emission control is in general required for the regional O3 pollution control.  相似文献   

16.
During the summer portion of the 1987 Southern California Air Quality Study (SCAQS), outdoor smog chamber experiments were performed on Los Angeles air to determine the response of maximum ozone levels, O3(max), to changes in the initial concentrations of hydrocarbons, HC, and nitrogen oxides, NOx. These captive-air experiments were conducted in downtown Los Angeles and in the downwind suburb of Claremont. Typically, eight chambers were filled with LA air in the morning. In some chambers the initial HC and/or NOx concentrations were changed by 25% to 50% by adding various combinations of a mixture of HC, clean air, or NOx. The O3 concentration in each chamber was monitored throughout the day to determine O3(max).An empirical mathematical model for O3(max) was developed from regression fits to the initial HC and NOx concentrations and to the average daily temperature at both sites. This is the first time that a mathematical expression for the O3-precursor relationship and the positive effect of temperature on O3(max) have been quantified using captive-air experiments. An ozone isopleth diagram prepared from the empirical model was qualitatively similar to those prepared from photochemical mechanisms. This constitutes the first solely empirical corroboration of the O3 contour shape for Los Angeles.To comply with the Federal Ozone Standard in LA, O3(max) must be reduced by approximately 50%. Several strategies for reducing O3(max) by 50% were evaluated using the empirical model. For the average initial conditions that we measured in LA, the most efficient strategy is one that reduces HC by 55–75%, depending on the ambient HC/NOx ratio. Any accompanying reduction in NOx would be counter-productive to the benefits of HC reductions. In fact, reducing HC and NOx simultaneously requires larger percentage reductions for both than the reduction required when HC alone is reduced. The HC-reduction strategy is the most efficient on average, but no single strategy is the optimum every day.  相似文献   

17.
为确定石家庄东部郊区交通干线附近O3生成光化学敏感性,利用2019年1月1日—2020年10月31日在线观测的NOx、NOy和O3等数据计算并分析了O3生成效率(OPE)及O3光化学敏感性的NOx临界浓度.结果表明:1交通干线附近O3光化学敏感性存在季节差异,春季主要受VOCs控制,整体OPE为2.6±0.3,夏、秋季节主要受NOx与VOCs协同控制,整体OPE分别为5.3±0.4和5.1±0.8;2NOx体积分数>11×10-9时,O3生成主要为VOCs控制;NOx体积分数介于6×10-9~11×10-9时,O3生成主要受VOCs与NOx协同控制;NOx体积分数<6×10-9时,O3生成主要为NOx控制;3O3生成敏感性存在日变化特征,10:00之前O3生成主要受VOCs控制,10:00—11:00是O3生成由VOCs控制转变为VOCs和NOx协同控制的过渡时段,12:00之后O3生成主要由VOCs和NOx协同控制,且午后14:00—16:00之间NOx对O3控制比例凸显.因此,石家庄O3治理不但要重视NOx与VOCs排放源的协同管控,尤其午后还需要对NOx排放源进行分时段精细化管控.  相似文献   

18.
Outdoor smog chamber experiments were used to study the sensitivity of the yields of two important nitrogen-containing pollutants, nitric acid (HNO3) and peroxyacetyl nitrate (PAN) to changes in nonmethane hydrocarbon (HC) and nitrogen oxide (NOx) concentrations in Los Angeles. The experiments were conducted at two sites in the Los Angeles Basin using eight chambers filled with morning Los Angeles air on 33 days. At least one chamber was unchanged and served as a control, while the initial HC and/or NOx concentrations were changed by 25–50% in up to seven chambers to simulate O3 control strategies and to broaden the range of HC - NOx conditions studied. Empirical models that predict the maximum yields of HNO3 and PAN were used to determine the response of these pollutants to three possible ozone control strategies. All three strategies (reductions in HC, NOx or both HC and NOx) reduced PAN while only NOx reductions decreased HNO3. However, reducing NOx increased the HC reductions required to attain lower O3 levels. Thus, there is a conflict between the O3 and HNO3 control strategies.  相似文献   

19.
A mational air quality monitoring network has been established in the U.K. by Warren Spring Laboratory, on behalf of the U.K. Department of the Environment, to determine compliance with the European Community Directive for nitrogen dioxide. Data from the six network sites for 1987 are presented and analysed.No site in the U.K. breached the NO2 Directive Limit Value during this year, though the closest approaches were at the two London stations. Annual average NO2 concentrations, which varied from 23 to 39 ppb, were consistent with the top five percentile of long-term measurements from a national survey of over 360 U.K. urban areas carried out in 1986.The temporal variability of NO2 concentrations was substantially lower over all time scales than that for NO: winter/summer ratios for all sites averaged 2.9 for NO and 1.3 for NO2. Most sites showed strong diurnal variations for NO which were primarily influenced by traffic emissions during rush hours, although these variations were less marked for NO2.A markedly non-proportional relationship between annual and daily average NO2 and NOx levels was observed, and this has important implications for its efficacy of possible NOx emission control strategies. An analysis of measured NO2/NOx ratios over weekends and weekday periods demonstrates, for instance, that a 20% emission cutback may result, typically, in a corresponding NO2 reduction of 12% at urban locations in the U.K. NOx reductions, however, exert a more proportional effect on NO2 concentrations at kerbside and rural locations.  相似文献   

20.
北京市大气光化学氧化剂污染研究   总被引:24,自引:3,他引:21  
根据在北京市开展的光化学氧化剂系列研究,讨论北京市主要光化学氧化剂O3,H2O2和有机过氧化物的污染浓度水平及其污染特征,探讨光化学氧化剂的形成机制及其主要影响因素。结果表明,北京市存在严重的光化学氧化剂污染,中关村大气臭氧(03)最大浓度不仅逐年递增,而O3最大值的出现时间也提前,说明大气光化学活性逐年增强。光化学烟雾的重要产物过氧化氢(H2O2)和甲基过氧化氢(MHP)的浓度水平较高,最大浓度分别为3.69和3.26ug/m3。日益严重的大气NOx污染为光化学氧化剂的生成提供了充足的前体物,北京市的大气污染己逐渐转为机动车尾气污染型,控制北京市光化学氧化剂污染的有效途径是降低NOx排放。   相似文献   

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