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1.
近年来近地面臭氧问题日益凸显,成为影响空气质量持续改善的瓶颈.本研究基于2017年8—9月在湖州市城区开展的为期1个月的臭氧及其前体物挥发性有机物(VOCs)和氮氧化物(NOx)在线观测数据,分析了臭氧及其前体物污染特征,利用正矩阵因子分析(PMF)解析了VOCs来源,并采用基于观测的模型(OBM)对臭氧生成机制进行研究.研究结果表明:1)观测期间湖州市VOCs平均体积分数为(24.78±9.10)×10-9,其中占比最高的组成为烷烃、含氧VOCs (OVOCs)和卤代烃;2)在臭氧非超标时段,湖州市臭氧生成处于VOCs控制区,而在臭氧重污染期间湖州市处于以VOCs控制为主的过渡区;3)在臭氧超标时段,对臭氧生成潜势(OFP)贡献最大的是芳香烃(39.6%),其次是烯烃(21.5%)和OVOCs (19.4%),排名前三的关键组分为甲苯、乙烯和间/对二甲苯;4)源解析结果显示观测期间湖州市VOCs的主要来源是溶剂使用(27.0%)、交通排放(22.7%)、背景+传输(19.3%)、工业排放(16.9%)、汽油挥发(7.7%)和植物排放(6.4%),重污染过程期间对OFP贡献最大的两类源是交通排放源和溶剂使用源,贡献百分比分别为35.1%和30.5%.因此,对交通排放和溶剂使用方面进行控制管理对湖州市大气臭氧污染防控有重要意义.  相似文献   

2.
Study of a high SO2 event observed over an urban site in western India   总被引:1,自引:0,他引:1  
Continuous measurements of SO2, NOx and O3 along with sampling based measurements of CO, CH4, NMHCs and CO2 were carried out during May, 2010 at Ahmedabad. The diurnal variations of SO2 in ambient air exhibited elevated values during the night and lower levels during the sunlit hours. The mean concentration of SO2 during the study period was 0.95 ± 0.88 ppbv. However, the ambient SO2 exceeded 17 ppbv in the night of 20 May, 2010. On the same day, tropospheric columnar SO2 from OMI showed almost 350% increase corroborating the surface observations over an extended height regime. This was also the highest columnar value of SO2 during the summer of 2010. Columnar loadings were also found to be high for formaldehyde, precipitable water vapor and aerosol optical depth on 20 May. Elevated concentrations were also recorded for other trace gases like NO2 and O3. Analysis of related data of trace gases indicated characteristics of fresh emissions with dominant contributions from mobile sources during the study period. However, SO2/NO2 ratio of 0.36 during the event period on 20th May connotes non-local influences. Analyses of meteorological parameters suggest combined impacts of transport and inversion causing higher levels of SO2 and other pollutants during 20?C21 May. Episodes of such enhancements may perturb chemical and radiative balance of the atmosphere.  相似文献   

3.
We have studied long-term changes in tropospheric NO2 over South India using ground-based observations, and GOME and OMI satellite data. We have found that unlike urban regions, the region between Eastern and Western Ghat mountain ranges experiences statistically significant decreasing trend. There are few ground-based observatories to verify satellite based trends for rural regions. However, using a past study and recent measurements we show a statistically significant decrease in NOX and O3 mixing ratio over a rural location (Gadanki; 13.48° N, 79.18° E) in South India. In the ground-based records of surface NOX, the concentration during 2010–11 is found to be lower by 0.9 ppbv which is nearly 60 % of the values observed during 1994–95. Small but statistically significant decrease in noon-time peak ozone concentration is also observed. Noon-time peak ozone concentration has decreased from 34?±?13 ppbv during 1993–96 to 30?±?15 ppbv during 2010–11. NOX mixing ratios are very low over Gadanki. In spite of low NOX values (0.5 to 2 ppbv during 2010–11), ozone mixing ratios are not significantly low compared to many cities with high NOX. The monthly mean ozone mixing ratio varies from 9 ppbv to 37 ppbv with high values during Spring and low values during late Summer. Using a box-model, we show that presence of VOCs is also very important in addition to NOX in determining ozone levels in rural environment and to explain its seasonal cycle.  相似文献   

4.
Connection between ozone concentration and atmosphere circulation is investigated based on measurements at BEO station, peak Moussala (2,925 m a.s.l.), for the period 09 August 2006 to 29 January 2008. Ozone concentration data are collected with UV-analyzer “Environnement O3 42” and meteo data with weather station “Vaisala”. There are measurements of 7Be. Data from NOAA HYSPLIT model for particle trajectories are also used. Eight wind directions and three ranges of wind velocities are employed in the analysis. A comparison of ozone concentrations in upward and downward air transport according to HYSPLIT model is made. The number of cases with ozone concentration above 63 ppb has been counted. Mann–Whitney nonparametric test is employed as a basic statistical method. Correlation between atmosphere pressure and tropospheric ozone content is made. The same is done for 7Be and ozone. The main conclusion is that there is not any local or regional pollution effect detectable at peak Moussala, but most of the ozone measured is due to emissions of hydrocarbons and NO x over a larger region. There could be some regional sources of ozone building substances in southwest direction from peak Moussala. Air transported from the north quarter has higher ozone concentrations compared to the south quarter. In vertical direction, upward transport of air masses shows higher values of ozone concentration. Higher wind velocity is associated with low ozone concentrations at peak Moussala. The annual course of ozone concentration has summer maximum and winter minimum. There is right connection between air pressure and ozone concentration. The same is valid for the correlation between 7Be and ozone. Diurnal ozone course shows daytime maximum in winter and nighttime maximum in summer.  相似文献   

5.
近年来武汉市臭氧污染日益严峻,成为影响空气质量达标的瓶颈,弄清臭氧及其前体物非线性关系是臭氧防控的关键和基础.本研究基于武汉中心城区2018年4—9月臭氧及其前体物在线观测数据,分析出武汉市臭氧浓度受前体物和气象条件等因素的共同影响,呈较为明显的季节变化和日变化特征.观测期间武汉市大气挥发性有机物(VOCs)平均体积分数为32.5×10-9,烷烃是武汉市VOCs的主要组分,其次是含氧VOCs (OVOCs)和卤代烃.利用基于观测的模型定量分析臭氧与前体物之间的关系,发现削减VOCs会引起臭氧生成潜势的显著下降,而削减氮氧化物则会使臭氧生成潜势升高,说明武汉市臭氧生成处于VOCs控制区.在人为源VOCs中,间/对二甲苯和邻二甲苯的相对增量反应活性(RIR)最高,是影响臭氧生成的关键组分.  相似文献   

6.
Measurements of NOx,y were made at Alert, Nunavut, Canada (82.5° N, 62.3° W) during surface layer ozone depletion events. In spring 1998, depletion events were rare and occurred under variable actinic flux, ice fog, and snowfall conditions. NOy changed by less than 10% between normal, partially depleted, and nearly completely depleted ozone air masses. The observation of a diurnal variation in NOx under continuous sunlight supports a source from the snowpack but with rapid conversion to nitrogen reservoirs that are primarily deposited to the surface or airborne ice crystals. It was unclear whether NOx was reduced or enhanced in different stages of the ozone depletion chemistry because of variations in solar and ambient conditions. Because ozone was depleted from 15–20 ppbv to less than 1 ppbv in just over a day in one event it is apparent that the surface source of NOx did not grossly inhibit the removal of ozone. In another case ozone was shown to be destroyed to less than the 0.5 ppbv detection limit of the instrument. However, simple model calculations show that the rate of depletion of ozone and its final steady-state abundance depend sensitively on the strength of the surface source of NOx due to competition from ozone production involving NOx and peroxy radicals. The behavior of the NO/NO2 ratio was qualitatively consistent with enhanced BrO during the period of active ozone destruction. The model is also used to emphasize that the diurnal partitioning of BrOx during ozone depletion events is sensitive to even sub ppbv variations in O3.  相似文献   

7.
Field measurement programs in Brazil during the dry seasons in August and September 1979 and 1980 have demonstrated the large importance of the continental tropics in global air chemistry. Many important trace gases are produced in large amounts over the continents. During the dry season, much biomass burning takes place, especially in the cerrado regions, leading to a substantial emission of air pollutants, such as CO, NO x , N2O, CH4 and other hydrocarbons. Ozone concentrations are enhanced due to photochemical reactions. The large biogenic organic emissions from tropical forests play an important role in the photochemistry of the atmosphere and explain why CO is present in such high concentrations in the boundary layer of the tropical forest. Carbon monoxide production may represent more than 3% of the net primary productivity of the tropical forests. Ozone concentrations in the boundary layer of the tropical forests indicate strong removal processes. Due to atmospheric supply of NO x by lightning, there is probably a large production of O3 in the free troposphere over the Amazon tropical forests. This is transported to the marine-free troposphere and to the forest boundary layer.  相似文献   

8.
传统的空气质量模型多使用简化的光化学反应机制来模拟大气污染物的形成.这些机制主要基于烟雾箱实验拟合的反应速率和产物来模拟二次产物(如臭氧(O3))前体物的氧化反应,具有一定的不确定性,导致模拟结果产生偏差.针对该问题,本研究将详细的大气化学机理(MCMv3.3.1)与美国国家环境保护局研制的第三代空气质量预报和评估系统CMAQ相结合(CMAQ-MCM),模拟研究长三角地区2015年8月27—9月5日臭氧高发时段的空气质量.CMAQ-MCM模型可以较好地模拟长三角地区6个代表城市O3和其前体物随时间的变化趋势.对模拟的O3日最大8 h平均浓度的统计分析表明,徐州表现最好(标准平均误差=-0.15,标准平均偏差=0.23).在长三角地区,居民源对挥发性有机物(VOCs)的贡献最大,占39.08%,其次是交通运输(33.25%)和工业(25.56%).能源对总VOCs的贡献最小,约为2.11%.对活性氧化氮(NOy)的分析表明,其主要组分是NOx(80%),其次是硝酸(HNO3)(<10%).O3的空间分布与NOy和NOx非常相似.HCHO等其他氧化产物的分布与NOx相似,这很可能是由于在高NOx条件下VOCs氧化产生的产物.甲基乙烯基酮(MVK)和甲基丙烯醛(MACR)的空间分布与自然源VOCs (BVOCs)非常相似,表明长三角地区MVK和MACR主要由BVOCs氧化生成.长三角地区受到人为源和自然源排放相互作用的影响.  相似文献   

9.
A seven-year record of surface ozone measurements from Denali NationalPark, Alaska shows a persistent spring maximum. These data, combined withmeasurements of NOx, hydrocarbons, O3, and PANfrom a continental site in Alaska during the spring of 1995 are used as thebasis for a sensitivity study to explore tropospheric photochemistry in thisregion. Because of the relatively high concentrations of NOx(mean of 116, median of 91 pptv), the net tendency was for photochemicalozone production. The range of net O3 production for averageconditions measured at this site during spring is between 0.96–3.9ppbv/day depending on the assumptions used; in any case, this productionmust contribute to the observed springtime maximum in O3.Model calculations showed that of the anthropogenic ozone precursors, onlyNOx had a strong effect on the rate of ozone production; themeasured concentrations of anthropogenic hydrocarbons did not significantlyaffect the ozone budget. Naturally produced biogenic hydrocarbons, such asisoprene, may also have a significant effect on ozone production, even atconcentrations of a few 10's of pptv. An observed temperature-isoprenerelationship from a boreal site in Canada indicates that isoprene may bepresent during the Alaskan spring. Measurements of isoprene taken duringthe spring of 1996 suggest that reactive biogenic hydrocarbon emissionsbegin before the emergence of leaves on deciduous trees and that theconcentrations were sufficient to accelerate ozone production.  相似文献   

10.
The objectives of this study were to identify species and levels of volatile organic compounds (VOCs), and determine their oxidation capacity in the rural atmosphere of western Senegal. A field study was conducted to obtain air samples during September 14 and September 15, 2006 for analyses of VOCs. Methanol, acetone, and acetaldehyde were the most abundant detected chemical species and their maximum mixing ratios reached 6 parts per billion on a volume basis (ppbv). Local emission sources such as firewood and charcoal burning strongly influenced VOC concentrations. The VOC concentrations exhibited little temporal variations due to the low reactivity with hydroxyl radicals, with reactivity values ranging from 0.001 to 2.6 s−1. The conditions in this rural site were rather clean. Low ambient NO x levels limited ozone production. Nitrogen oxide (NO x ) levels reached values less than 2 ppbv and maximum VOC/NO x ratios reached 60 ppbvC/ppbv, with an overall average of 2.4 ± 4.5 ppbvC/ppbv. This indicates that the rural western Senegal region is NO x limited in terms of oxidant formation potential. Therefore, during the study period photochemical ozone production became limited due to low ambient NO x levels. The estimated ozone formation reactivity for VOCs was low and ranged between −5.5 mol of ozone/mol of benzaldehyde to 0.6 mol/mol of anthropogenic dienes.  相似文献   

11.
During the summer (8 June through 3 September) of 2008, 9 ozone profiles are examined from Dakar, Senegal (14.75°N, 17.49°W) to investigate ozone (O3) variability in the lower/middle troposphere during the pre-monsoon and monsoon periods. Results during June 2008 (pre-monsoon period) show a reduction in O3 concentrations, especially in the 850–700 hPa layer with Saharan Air Layer (SAL) events. However, O3 concentrations are increased in the 950–900 hPa layer where the peak of the inversion is found and presumably the highest dust concentrations. We also use the WRF-CHEM model to gain greater insights for observations of reduced O3 concentrations during the monsoon periods. In the transition period between 26 June and 2 July in the lower troposphere (925–600 hPa), a significant increase in O3 concentrations (10–20 ppb) occur which we suggest is caused by enhanced biogenic NOX emissions from Sahelian soils following rain events on 28 June and 1 July. The results suggest that during the pre-monsoon period ozone concentrations in the lower troposphere are controlled by the SAL, reducing ozone concentrations through heterogeneous chemical processes. At the base of the SAL we also find elevated levels of ozone, which we attribute to biogenic sources of NOX from Saharan dust that are released in the presence of moist conditions. Once the monsoon period commences, lower ozone concentrations are observed and modeled which we attribute to the dry deposition of ozone and episodes of ozone poor air that is horizontally transported into the Sahel from low latitudes by African Easterly Waves (AEWs).  相似文献   

12.
The CHIMERE mesoscale chemistry transport model is used for the quantitative assessment of the contribution of transboundary transport of anthropogenic admixtures from China to the surface concentrations of major suspended pollutants, aerosol PM10, ozone O3, and nitrogen oxides NOx in the Far Eastern region. Analyzed in detail are the time series of concentration of mentioned substances computed with the model taking account and not taking account of anthropogenic emissions in China. It is revealed that the transboundary transport of anthropogenic pollutants can cause the recurring episodes of manyfold increase in the concentration of PM10 in the south of Khabarovsk region, as well as more rare variations of O3 and NOx concentration. The trajectory and synoptic analysis demonstrated that the episodes of the increase in the concentration of PM10 and O3 in the south of the region mainly depend on the carryover of air masses from northeastern China in the front part of continental cyclones.  相似文献   

13.
The mixing ratios for ozone and NOx (NO+NO2) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NOx levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NOx from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NOx mixing ratio. For NOx mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NOx]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NOx]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O3 in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NOx levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NOx]0.2 ppbv, 0.3 ppbv[NOx]0.7 ppbv and 1 ppbv[NOx]. These monthly ozone averages reflect the seasonal ozone dependence on the NOx level.  相似文献   

14.
By means of a three-dimensional meteorological model (MM5) and a chemical model,the distributions of tropospheric ozone and its precursors over China have been simulated in summer and winter time,16-18 August 1994 and 7-9 January 1995.The distribution of ozone over the Tibetan Plateau in summer time is deeply discussed.The simulated results indicate that thedistributions of surface ozone and NOx are in good agreement with observed results,and human activities and photochemical reactions are the main factors controlling the surface ozone and NOx concentrations.In addition,higher ozone concentrations are coincided with the air convergence,and the lower concentrations are related to the air divergence.In summer,over the Tibetan Plateau the strong flow convergence results in higher ozone concentrations in the lower troposphere:and the strong flow divergence results in lower ozone concentrations in the upper troposphere.In winter time ozone concentrations show large-scale characteristics controlled by westerly flow,and in the jet area they are lower than those outside the jet.  相似文献   

15.
The response of tropospheric ozone to a change in solar UV penetration due to perturbation on column ozone depends critically on the tropospheric NO x (NO+NO2) concentration. At high NO x or a polluted area where there is net ozone production, a decrease in column ozone will increase the solar UV penetration to the troposphere and thus increase the tropospheric ozone concentration. However, the opposite will occur, for example, at a remote oceanic area where NO x is so low that there is net ozone destruction. This finding may have important implication on the interpretation of the long term trend of tropospheric ozone. A change in column ozone will also induce change in tropospheric OH, HO2, and H2O2 concentrations which are major oxidants in the troposphere. Thus, the oxidation capacity and, in turn, the abundances of many reduced gases will be perturbed. Our model calculations show that the change in OH, HO2, and H2O2 concentrations are essentially independent of the NO x concentration.  相似文献   

16.
Ozone Concentrations in Rural Regions of the Yangtze Delta in China   总被引:4,自引:0,他引:4  
Elevated concentrations of ozone have been observed at six non-urban, surface monitoring sites in the Yangtze Delta of China during a 16-month field experiment carried out in 1999 and 2000 as part of the joint Chinese-American China-MAP Project (the Yangtze Delta of china as an Evolving Metro-Agro-Plex). The average daytime (0900–1600 h) ozone levels for the monitoring period at sites ranged from 35 to 47 ppbv (parts per billion by volume) and the mean ozone levels from 26 to 35 ppbv. Observed data show seasonal variation obviously, with highest mixing ratios of ozone in May. Average daytime ozone levels in May at sites were between 60 and 79 ppbv. High ozone concentrations were most prevalent during the late spring. Frequency counts of hourly mean ozone concentration over 60 ppbv and 40 ppbv appeared peak values of 22–39% and 42–74% in May at sites. Even higher daytime ozone levels were observed during two regional episodes, in which average daytime (0900–1600 h) ozone concentrations during 10 May and 23 May 2000 were 68 to 81 ppbv, during Oct. 18 and Oct. 28, 1999 were 59 to 67 ppbv at sites. Peak value of ozone mixing ratio appearing in late spring, instead of in summer, was attributed to summer monsoon. Backward trajectories showed that ozone episodes associated with meteorological conditions. Also many high ozone levels associated with high CO levels and high CO to NO x ratios, which suggests a contribution from sources of emission involving incomplete combustion.  相似文献   

17.
NO, NOx, NOy and O3 have been measuredduring the airborne EXPRESSO experiment, November 96,which took place near Bangui (Central Africa) at thebeginning of the dry season. This period correspondsto an intense burning activity. Chemical andphotochemical characteristics of the planetaryboundary layer, which corresponds most of the time tothe monsoon layer, and the Harmattan layer, which issituated above the latter, have been studied forsavanna as well as rain forest areas. These two layersare very different when considering the chemicalcomposition (especially for ozone and NOz) andthe photochemical age.The relationship of photochemical ozone productionversus photochemical NOx oxidation products hasbeen investigated. Results indicate an ozoneproduction efficiency (OPE) ranging from 6.3 to 14.8in the planetary boundary layer. Thus, this layer ischaracteristic of a photochemically young and activeair mass. In this layer, the ozone potentialproduction increases with the air mass photochemicalage. On the other hand, the Harmattan layer shows anOPE ranging from 4.6 to 7.4. These values arecharacteristic of photochemically well-aged airmasses. In this layer, the ozone potential productionseems to be exhausted with values around 4.0 (i.e., 4ozone molecules produced for each NOx moleculeemitted).  相似文献   

18.
A 2-D global chemistry-transport model is set up in this paper.The model simulates the atmospheric ozone distributions well with specified dynamical conditions.The analysis of ozone variation mechanism shows that ozone is chemically in quasi-equilibrium except for the polar night region where the variation of ozone concentration is under the control of dynamical processes,that the oxygen atoms which produce ozone are mainly provided by the photolysis of O2 in the upper stratosphere and by the photolysis of NO2 in the lower stratosphere and the troposphere.and that the ozone is destroyed mainly by NOx:the reactions between NOx and O3 and the odd oxygen cycle contribute 80% to more than 90% of the ozone destruction.  相似文献   

19.
In this study, we used satellite data (GOME and MOPITT) together with a global chemical-transport-model of atmosphere (MOZART-2) to characterize the chemical/aerosol composition over eastern China. We then estimated the effects of local emissions in China on the chemical budgets in other regions of the world. Likewise, we also investigated the effects of air pollution from other regions on the chemical budget over eastern China. The study shows that the column CO and NO x concentrations are also high in eastern China. The high CO and NO x concentrations produce modest levels of O3 concentrations during summer (about 40 to 50 ppbv) and very low O3 during winter (about 10 to 20 ppbv) in eastern China. The calculated NO2 column is fairly consistent from the GOME measurement. The calculated CO column is underestimated from the MOPITT measurement. One of the reasons of the underestimation of the predicted CO is due to a fact that the CO emissions were taken without considering the rapid increase of emissions from 1990 to 2000. The calculated surface O3 is consistent with the measured values, with strong seasonal variations. However, the measurement is very limited, and more measurements in eastern China will be needed. The column NO2 has a very strong seasonal variation in eastern China, with the highest concentrations during winter and the lowest concentrations during summer. The cause of this seasonal variability is mainly due to the seasonal changes in the chemical loss of NO x , which is very high in summer and very low during winter. The effects of the local emissions in China and long-range transport from other regions on the chemical distributions in eastern China are studied. The results show that NO x concentrations in eastern China are mostly caused by the local emissions in China, especially during the winter. The CO concentration over eastern China is from both the local emissions (30% to 40%) and the transport from other regions. Likewise, the CO emissions in China have an important effect on the other regions of the world, but the effect is limited in the northern hemisphere. The local emissions in China also have an important effect on surface O3 concentrations. During winter, the local emissions reduce the surface O3 concentrations by 30 to 50%. During summer, the local emissions produce about 50 to 70% of the O3 concentration in eastern China.  相似文献   

20.
Simultaneous ozone measurements were made at a rural site, 25 km SSW of the city of Jerusalem, and in the center of the city during a period of 28 months. The ozone data were supplemented by SO2, NO/NO x ,and meteorological measurements at both sites. Elevated ozone concentrations were recorded at the rural site, mostly during the spring months (May and June) during which the monthly averages and the monthly averages of the daily 30 min maximum levels equalled those measured in the city. During the summer months, both average and peak levels were lower at the rural site by 20 and 35 ppb. The increased ozone levels at the rural site were accompanied by a parallel increase of SO2 and NO x ,suggesting hat the excess ozone at the rural site is a result of a transformation during transport of air pollutants from coastal sources.  相似文献   

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