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1.
The ozone concentration near the earth's surface has been measured at some stations in the GDR for more than 30 yr using the wet chemical method. Even at rural stations the ozone data show a significant linear increase by about 1–3% yr–1. The ozone increase being stronger in summer than in winter is assumed to be due to photochemical ozone production from increasing anthropogenic emissions of trace gases that are transported over long distances. A weaker ozone increase by only about 0.2% per year was observed in the free troposphere (5.5 km) from balloon-soundings at Lindenberg within the period 1975–1984. If the ozone trends continue, the ozone concentration near the surface and its seasonal amplitude will have doubled around the turn of the century as compared to the mid-fifties.  相似文献   

2.
The concentration of gas-phase peroxides has been measured almost continuously at the Cape Grim baseline station (41° S) over a period of 393 days (7702 h of on-line measurements) between February 1991 and March 1992. In unpolluted marine air a distinct seasonal cycle in concentration was evident, from a monthly mean value of>1.4 ppbv in summer (December) to <0.2 ppbv in winter (July). In the summer months a distinct diurnal cycle in peroxides was also observed in clean marine air, with a daytime build-up in concentration and decay overnight. Both the seasonal and diurnal cycles of peroxides concentration were anticorrelated with ozone concentration, and were largely explicable using a simple photochemical box model of the marine boundary layer in which the central processes were daytime photolytic destruction of ozone, transfer of reactive oxygen into the peroxides under the low-NOx ambient conditions that favour self-reaction between peroxy radicals, and continuous heterogeneous removal of peroxides at the ocean surface. Additional factors affecting peroxides concentrations at intermediate timescales (days to a week) were a dependence on air mass origin, with air masses arriving at Cape Grim from higher latitudes having lower peroxides concentrations, a dependence on local wind speed, with higher peroxides concentrations at lower wind speeds, and a systematic decrease in peroxides concentration during periods of rainfall. Possible physical mechanisms for these synoptic scale dependencies are discussed.  相似文献   

3.
Detailed studies have been made of the behaviour of gases and radicals involved in the production of oxidants at the Weybourne Atmospheric Observatory in both summertime and wintertime conditions. In June 1995 the range of meteorological conditions experienced varied such that ozone destruction was observed in clean northerly air flows reaching Weybourne down the North Sea from the Arctic, and ozone production was observed in varying degrees in air with different loadings of nitrogen oxides and other precursors. The transition point for ozone destruction to ozone production occurred at a nitric oxide concentration of the order of 50 pptv. Plumes of polluted air from various urban areas in the U.K. were experienced in the June campaign at Weybourne. Quantitative studies of ozone production in a plume from the Birmingham conurbation on 18 June 1995 showed that the measurement of ozone production agreed well with calculated production rates from the product of the nitric oxide and peroxy radical concentrations (r2=0.9). In wintertime conditions (October–November 1994) evidence was also found for oxidant production, defined as the sum of O3+NO2. At this time of year the peroxy radical concentrations (RO2) were much lower than observed in the summertime and the nitric oxide (NO) was much higher. There was still sufficient RO2 during the day, however, for a slow accumulation of oxidant. Confirmatory evidence for this comes from the diurnal co-variance of (O3+NO2) with PAN, an excellent tracer of tropospheric photochemistry. The same type of covariance occurs in summer between PAN and ozone. The results obtained in these series of measurements are pertinent to understanding the measures necessary to control production of regional photochemical air pollution, and to the production of ozone throughout the northern hemisphere in winter.  相似文献   

4.
我国北方地区对流层中下层臭氧收支   总被引：1，自引：0，他引：1       下载免费PDF全文
为了揭示我国北方地区对流层中下层臭氧(O3) 的形成机理以及周边地区的污染输送对我国北方地区对流层中下层O3收支的影响, 在与外场观测数据比较分析的基础上, 利用全球化学输送模式(MOZART-2) 采用收支分析方法定量分析了影响我国北方地区对流层中下层O3的各个物理化学过程。结果表明:我国北方地区对流层下层O3最重要的来源是光化学生成作用, 约占总来源的58.3%(41.5 Tg), 光化学生成反应中HO2对于O3生成的贡献最大; 最大的汇是干沉降过程, 约占总汇的43.2%(26.2Tg); 水平净输送作用对我国北方地区对流层中下层O3收支的影响非常大, 在我国北方地区对流层下层, 41.6%左右的O3来自水平净输送, 随高度增加, 水平输送影响增大, 我国北方地区对流层中层大约81.5%的O3来自水平净输送。  相似文献   

5.
The analysis of surface ozone variability requires besides chemicalstudies the consideration of meteorological conditions and dynamicprocesses. Our research focuses on the mechanisms in connection with coldfront passages. A statistical study and case studies of cold front passageswere carried out at six German ground-based sites during the year 1990.After the passage of cold fronts three typical developments of thenear-ground ozone concentrations could be identified. Usually the ozoneconcentrations decrease due to advection of clean air masses or due toenhanced cloudiness preventing the photochemical production of ozone,chemical destruction by nitrogenoxides, and heterogeneous chemistry. In somecases the concentrations increased by reason of downward mixing of ozoneenriched air intruded from the stratosphere into the troposphere bytropopause foldings. For a few cases no modification set in. The decreasewas mostly twice as strong as the increase. The latter was between 4 and 8ppb on the average. Special emphasis is given to the transport ofstratospheric ozone down to the ground. There is no direct evidence forstratospheric ozone at ground level, because it cant be distinguished fromthe tropospheric one, but from case studies circumstantial evidence is foundin favour of it. As an example of increasing ozone behind the passage ofcold fronts one case study typical of all other case studies is presented.It shows the characteristic properties of the corresponding fronts, whichare fast movement, a vertical split structure and strong convection.  相似文献   

6.
利用2015—2019年中国东部20个省份222个城市的地面O_3观测数据和全球再分析风场数据,研究了中国东部地区O_3的时空分布特征,以及在亚洲夏季风背景下污染上风方O_3光化学输送对下风方O_3质量浓度季节变化的影响。结果表明:中国东部地区O_3质量浓度夏季高、冬季低,O_3质量浓度按照东南、华东、东北、华北的顺序依次升高,位于中高纬度的华北、东北地区明显高于位于中低纬度的华东、华南地区。不同城市、不同季节O_3质量浓度日变化形态具有较好的一致性,都表现为夜晚低、清晨逐渐升高、下午至黄昏达到最大的单周期变化形态,具有典型的光化学控制特征。春季,亚洲夏季风开始影响中国东部地区,华东、华北、东北地区为大范围的O_3高值区;夏季,亚洲夏季风将O_3及其前体物由纬度较低的华南、华东地区向纬度较高的华北、东北地区不断输送和累积,并在夏季强紫外辐射作用下发生光化学反应,导致夏季华北、东北地区的O_3污染。  相似文献   

7.
Ozone photochemical production and loss in very different environments at Waliguan baseline station and Lin'an background station were simulated by using the measurement data and photochemical box model.The results show that net ozone photochemical production rate is negative,about 0.5 ppb/d,at Waliguan baseline sation,because of very low precursor concentrations.But at Lin'an background station,the net photochemical ozone production is positive,about 2-3 ppb/h.which is very closed with the measurement at Lin'an.That means ozone production was controlled by photochemical reactions at Lin'an background station,because of the higher precursor concentrations.The net destruction rate,at Waliguan Mt.,is not large,so that future increase in anthropogenic emission of reactive nitrogen will lead to larger production rates of steady-state O3 concentration.  相似文献   

8.
The comparison is represented of the results of surface ozone concentration measurements in two megalopolises, Moscow and Kiev. A temporal course of ozone concentration and temperature in both cities is close by the shape and is typical of medium-polluted plain stations. In both megalopolises, two maxima are observed within the seasonal ozone concentration variability, in spring and summer, and during the day, a usual ozone concentration maximum (approximately in 2–3 hours after the local noon) and the night one being typical of big cities. An average ozone concentration and an average temperature in corresponding periods are higher in Kiev than in Moscow. Evidently, the summer maximum is associated with photochemical ozone generation processes, and the spring one, with dynamic processes of its transport in the atmosphere. In both megalopolises, the episodes are observed in the warm period under meteorological conditions being unfavorable for the pollutant scattering in the atmosphere when the ozone concentration exceeds the threshold limit value and is dangerous for health. The repeatability of such episodes is the highest one in July-August. In Kiev, such episodes are more frequent than in Moscow. An effective statistical model is constructed for both megalopolises in which the observed ozone concentration is represented in the form of regression function of temperature and relative humidity.  相似文献   

9.
NUMERICAL SIMULATION OF THE FORMATION MECHANISM OF THE ANTARCTIC OZONE HOLE   总被引：1，自引：0，他引：1  
The global zonally averaged atmospheric chemistry model is developed in this paper.Theformation mechanism of the Antarctic ozone hole is numerically simulated using the model to checkthe viewpoints on the formation mechanism.The results show that:(1)The Antarctic ozone hole is a special phenomenon resulting from the heterogeneousreactions on the surface of the polar stratospheric cloud particles,under the special conditions oftemperature and circulation in Antarctic spring.The heterogeneous reactions reduce the NO_2concentration,resulting in the decrease of ozone production rate.The ozone content decreaseswhen its production is less than its destruction.This is the direct cause for the formation of theAntarctic ozone hole.(2)The impact of the polar vortex on the transport of trace species is not the determinativefactor in the formation of the Antarctic ozone hole.but makes the intensity of the ozone holechanged.(3)The solar cycles have negligible influence on the intensity of the Antarctic ozone holethrough photochemical reactions.  相似文献   

10.
Measurements of the sum of peroxy radicals [HO2 + RO2],NOx (NO + NO2) and NOy (the sum of oxidisednitrogen species) made at Mace Head, on the Atlantic coast of Ireland in summer 1996 and spring 1997 are presented. Together with a suite of ancillary measurements, including the photolysis frequencies of O3 O(1D)(j(O1D)) and NO2 (j(NO2)), the measured peroxy radicals are used to calculate meandailyozone tendency (defined as the difference of the in-situphotochemical ozone production and loss rates); these values are compared with values derived from the photochemical stationary state (PSS) expression. Although the correlation between the two sets of values is good, the PSS values are found to be significantly larger than those derived from the peroxy radical measurements, on average, in line with previous published work. Possible sources of error in these calculations are discussed in detail. The data are further divided up into five wind sectors, according to the instantaneous wind direction measured at the research station. Calculation of mean ozone tendencies by wind sector shows that ozone productivity was higher during spring (April–May) 1997 than during summer (July–August) 1996across all airmasses, suggesting that tropospheric photochemistry plays an important role in the widely-reported spring ozone maximum in the Northern Hemisphere. Ozone tendencies were close to zero for the relatively unpolluted south-west, west and north-west wind sectors in the summer campaign, whereas ozone productivity was greatest in the polluted south-east sector for both campaigns. Daytime weighted average ozone tendencies were +(0.3± 0.1) ppbv h–1 for summer 1996 and +(1.0± 0.5) ppbvh–1 for spring 1997. These figures reflect the higher mixing ratios of ozone precursors in spring overall, as well as the higher proportion of polluted air masses from the south-east arriving at the site during the spring campaign. The ozone compensation point, where photochemical ozone destruction and production processes are in balance, is calculated to be ca. 14 pptv NO for both campaigns.  相似文献   

11.
利用东亚清洁背景站近地面臭氧观测资料,结合风场和降水资料,分析东亚各地区臭氧的多年季节变化特征,并探讨东亚太平洋地区臭氧的季节和年际变化与季风的关系以及影响近地层臭氧的主要因子。结果表明：东亚大部分地区与北半球背景站观测一致,近地层臭氧季节变化表现为春季最高、夏季最低的特征;但在东亚中纬度33～43°N,臭氧表现为夏季最高,而在东亚20°N以南地区臭氧则表现为冬末、春初最高。东亚太平洋沿岸近地面臭氧的季节变化主要受东亚冬、夏季风环流的季节变化控制。该地区不同纬度上春季峰值出现时间的差异与亚洲大陆春季不同时期污染物输送路径的差异有关。对东亚太平洋沿岸对流层顶附近位势涡度、高空急流和垂直环流季节变化的分析表明,冬春季可能是平流层向对流层输送的最强期,对近地面臭氧贡献最大。初夏至秋季（5-11月）,平流层向对流层输送较弱,对近地面臭氧贡献较小。东亚太平洋地区夏季风爆发的时间和强度以及季风环流型的年际差异是导致该地区春、夏季臭氧年际变化的主要原因;而季风降水和云带位置以及平流层一对流层交换是造成臭氧年际变化的其他原因。  相似文献   

12.
Turbulent fluxes of sensible and latent heat and ozone were measured aboard a German Aerospace Research Establishment motorglider over the Swiss Plateau during the first field experiment of the Swiss air pollution experiment POLLUMET. In the lower part of the boundary layer, the ozone fluxes are negative (downward) throughout the day as a result of deposition and photochemical destruction at the surface. In the upper part of the boundary layer, the ozone fluxes tend to be negative until mid-afternoon and then become positive. The change in sign occurs after the ozone concentration in the boundary layer exceeds that in the reservoir above the inversion. Downdrafts bringing air parcels with ozone deficits across the inversion then become major contributors to the flux. The positive fluxes at upper levels result in an increase in flux divergence in mid-afternoon that is balanced by a relatively large source term in the ozone concentration budget.  相似文献   

13.
Ozone episodes (> 100 ppbv) were observed frequently in Jinan, an urban site located between the highly polluted Yangtze Delta and Beijing–Tianjin region in East China. In this study, the ozone episodes observed in 2004 were analysed using the Hybrid Single-particle Lagrangian Integrated Trajectory (HYSPLIT) model and surface meteorological data, as well as Air Pollution Index (API). The meteorological conditions of episode days and non-episode days were compared and examined, and categorization of 6 groups of backward trajectories was performed. The results show that, most episodes were caused by local photochemical production (e.g., induced by sufficient sunshine duration and high temperature) and pollutant accumulation (e.g., induced by little rainfall and low wind speed), and transport of pollutants from the highly polluted regions could significantly influence the air quality at the site, especially from Yangtze Delta region. In addition, three typical ozone episodes were analysed using HYSPLIT model to infer any long-distance transport and surface meteorological data to infer the local ozone production potential. At last, the functions and inadequacies about the usage of HYSPLIT model combined with surface meteorological data for the analysis of photochemical pollution were discussed.  相似文献   

14.
利用南极大陆沿岸中山站2008-2013年的地面臭氧连续观测数据和相关资料,对地面臭氧损耗事件（ODE）进行研究。结果显示,春季南极中山站常发生臭氧损耗事件。在该事件发生期间,气象要素有明显的突变过程,包括气温明显下降,风向由偏东风转变为偏北风,风速随之下降。来自海冰区的偏北风增多,风速很小,使臭氧浓度维持在较低水平。地面臭氧损耗事件主要与南极沿岸海冰区的活性溴（BrO）浓度有关。春季南极大陆沿岸海冰冻融过程中形成的冰间水道和冰间湖,在低温的作用下会再次冻结,形成薄冰和霜花。卫星资料能够观测到薄冰区释放的活化海盐溴高浓度区,活性溴与臭氧发生化学反应形成地面臭氧损耗事件。臭氧损耗现象是在未受到人为影响的自然状态下发生的,与中高纬度地区光化学反应导致臭氧消耗有所不同。   相似文献   

15.
The integrated assessment of the influence of air mass transport directions on the average long-term seasonal variations of concentrations of minor gas components (MGC: ozone, CO, NO2) of the atmosphere is carried out according to the data of a number of European stations. Distributions of nitrogen dioxide and carbon monoxide concentrations according to transport directions are similar to each other and differ considerably from the distribution of ozone concentrations. It is demonstrated that the relationships of levels of spring and summer ozone concentrations maxima differ considerably at all examined stations in different regions of Europe depending on different transport directions: the summer maximum is stronger pronounced according to the data for the southern and eastern directions than according to the data for the northern and western directions. The change of air transport directions may account for from 10% (Moscow region) to 30–40% (the northwest of continental Europe and Ireland) variations of MGC concentration. The obtained results point out the perspective of their use in statistical models of the forecast of MGC concentrations.  相似文献   

16.
2013年6—9月在河北省固城站观测到多次夜间对流性天气伴随地面O3混合比快速抬升的过程,并引起次日清晨到中午O3混合比升高。大多数对流过程中,O3混合比在半小时内升高至60×10-9～80×10-9,同时NOx等反应性气体混合比下降,θse值降低,说明下沉气流将高空气团带到地面,造成了O3混合比的升高。通过再分析资料得到下沉气团基本来源于对流层中下层,这一结论与当地进行的一次飞机观测结果吻合。多数对流过程中固城站和北京城区地面O3混合比和θse值有相同的变化趋势和程度。根据观测结果,推测华北地区在夏季和初秋时,对流层中下层存在O3高值区,混合比约为60×10-9～80×10-9。对流性天气对地面O3抬升的影响区域与对流系统的影响范围有关,可达到中尺度范围。华北地区光化学污染严重,对流性天气引起的地面O3混合比抬升程度比较强,对环境的影响值得关注。  相似文献   

17.
In this paper we try to identify and describe the specifics of the Berlin city plume characterised by a zone of enhanced photochemical activity downwind of the urban area, where the major emissions of ozone precursors (NOx and VOC) take place. Two Eulerian CTM systems (EURAD and REM3/CALGRID) and one Euler–Lagrangian model (LaMM5) are applied to thearea of Berlin/Brandenburg to investigate the processes involved in the evolution of the Berlin plume inherent to the models. The study focuses on 20 July 1998,the first special observation period (SOP) during BERLIOZ. The examination includes (1) the role of turbulence and transport and the role of mass flux to the surface during the evolution of the plume, (2) the import situation of the ground based measurement sites, (3)the terms of the ozone budget equation and their contribution to precursor distribution and ozone formation, (4) the substructures of the plume defined by its chemical regimes. Main results show that the complex meteorological conditions during this SOP with considerable turbulent transports demand an Euler–Lagrangian approach to determine the source receptor relationshipsfor the ground based measurement sites. These relations reveal that only a minor part (5%) of the air approaching Pabstthum and the more downwind (north-western) stations origins from Berlin and that the mutual transport between all sites was limited. The latter result afflicts the joint interpretation of data from different stations because the presumption to measure the same air mass is violated in many cases for this SOP. The CTM results reveal that the local net production of ozone within the plume was controlled by transport ad chemical processes both owning the same importance but tending to counteract each other. At this SOP far distance sources of ozone precursors originating from the Bohemian basin did not interfere the Berlin city plume although they generally have the potential to do so.  相似文献   

18.
城市化已引起大量痕量气态污染物、气溶胶以及臭氧前体物的人为排放,从而引起区域大气化学循环的扰动变化。在分析国内外研究现状与观测实例的基础上,进一步用辐射模式与化学模式研究了气溶胶对到达地面的光化辐射通量以及臭氧形成的影响,表明气溶胶可显著减小到达地面的光化学辐射通量,减缓光化学反应进程,并进一步抑制臭氧的形成;在目前广州等大城市的污染过程中,高浓度的气溶胶可造成光化学辐射通量衰减高达70%~80%,紫外线的衰减比可见光更明显,在可见光波段随波长增大衰减幅度减小,气溶胶层的存在对短波长激发的光化学过程的影响更加显著。分析说明城市污染大气中光化学反应的生成物与反应物之间存在自抑制过程,在目前的城市群复合污染情况下,气溶胶与臭氧之间的非线性相互作用值得关注。  相似文献   

19.
The seasonal and diurnal variations of ozone mixing ratios have been observed at Niwot Ridge. Colorado. The ozone mixing ratios have been correlated with the NO x (NO+NO2) mixing ratios measured concurrently at the site. The seasonal and diurnal variations in O3 can be reasonably well understood by considering photochemistry and transport. In the winter there is no apparent systematic diurnal variation in the O3 mixing ratio because there is little diurnal change of transport and a slow photochemistry. In the summer, the O3 levels at the site are suppressed at night due to the presence of a nocturnal inversion layer that isolated ozone near the surface, where it is destroyed. Ozone is observed to increase in the summer during the day. The increases in ozone correlate with increasing NO x levels, as well as with the levels of other compounds of anthropogenic origin. We interpret this correlation as in-situ or in-transit photochemical production of ozone from these precursors that are transported to our site. The levels of ozone recorded approach 100 ppbv at NO x mixing ratios of approximately 3 ppbv. Calculations made using a simple clean tropospheric chemical model are consistent with the NO x -related trend observed for the daytime ozone mixing ratio. However, the chemistry, which does not include nonmethane hydrocarbon photochemistry, underestimates the observed O3 production.  相似文献   

20.
A photochemical box model has been used to simulate the mixing ratio ofozone under conditions reflecting those encountered in the marine boundarylayer at Cape Grim, Tasmania, where a decade-long record of ozone mixingratio is available. The model is based on the proposition that ozone loss byphotolysis, atmospheric reaction with hydroperoxy and hydroxyl radicals, andsurface deposition is balanced by ozone gain via entrainment from the lowerfree troposphere with a small additional source in summer from photolysis ofnitrogen dioxide. This model simulates very well the observed ozone records,reproducing both the small diurnal cycle in ozone mixing ratio observedduring the summer months, and the factor of two seasonal ozone cycle showinga distinct winter maximum and summer minimum. The model result confirms thatunder the low-NOx conditions of the clean marine boundarylayer net photochemical loss of ozone occurs at all times of year.  相似文献   

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