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1.
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   

2.
Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH4 and NO x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO x emissions during this period while the contribution of CH4 to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.  相似文献   

3.
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   

4.
A one-dimensional photochemical model was used to explore the role of chlorine atoms in oxidizing methane and other nonmethane hydrocarbons (NMHCs) in the marine troposphere and lower stratosphere. Where appropriate, the model predictions were compared with available measurements. Cl atoms are predicted to be present in the marine troposphere at concentrations of approximately 103 cm-3, mostly as a consequence of the reaction of OH with HCl released from sea spray. Despite this low abundance, our results indicate that 20 to 40% of NMHC oxidation in the troposphere (0–10 km) and 40 to 90% of NMHC oxidation in the lower stratosphere (10–20 km) is caused by Cl atoms. At 15 km, NMHC-Cl reactions account for nearly 80% of the PAN produced.The model was also used to test the longstanding hypothesis that NOCl is an intermediate to HCl formation from sea salt aerosols. It was found that the NOCl concentration required (10 ppt) would be incompatible with field observations of reactive nitrogen and ozone abundance. Chlorine nitrate (ClONO2) and methyl nitrate (CH3ONO2) were shown to be minor components of the total NO y abundance. Heterogeneous reactions that might enhance photolysis of halocarbons or convert ClONO2 to HOCl or Cl2 were determined to be relatively unimportant sources of Cl atoms. Specific and reliable measurements of HCl and other reactive chlorine species are needed to better assess their role in tropospheric chemistry.  相似文献   

5.
A global two-dimensional (altitude-latitude) chemistry transport model is used to follow the changes in the tropospheric distribution of the two major radiatively active trace gases, methane and ozone, following step changes to the sustained emissions of the short-lived trace gases methane, carbon monoxide and non-methane hydrocarbons. The radiative impacts were dependent on the latitude chosen for the applied change in emissions. Step change global warming potentials (GWPs) were derived for a range of short-lived trace gases to describe their time-integrated radiative forcing impacts for unit emissions relative to that of carbon dioxide. The GWPs show that the tropospheric chemistry of the hydrocarbons can produce significant indirect radiative impacts through changing the tropospheric distributions of hydroxyl radicals, methane and ozone. For aircraft, the indirect radiative forcing impact of the NO x emissions appears to be greater than that from their carbon dioxide emissions. Quantitative results from this two-dimensional model study must, however, be viewed against the known inadequacies of zonally-averaged models and their poor representation of many important tropospheric processes.  相似文献   

6.
The Pacific Atmospheric Sulfur Experiment (PASE) was a field mission that took place aboard the NCAR C-130 airborne laboratory over the equatorial Pacific Ocean near Christmas Island (Kirimati, Republic of Kiribati) during August?CSeptember, 2007. Eddy covariance measurements of the ozone fluxes at various altitudes above the ocean surface, along with simultaneous mapping of the horizontal gradients provided a unique opportunity to observe all of the dynamical components of the ozone budget in this remote marine environment. The results of six daytime and two sunrise flights indicate that vertical transport into the marine boundary layer from above and horizontal advection by the tradewinds are both important source terms, while photochemical destruction consisting of 82% photolysis (leading to OH production), 11% reaction with HO2, and 7% reaction with OH provides the main sink. The overall photochemical lifetime of ozone in the marine boundary layer was found to be 6.5 days. Ocean uptake of ozone was observed to be fairly slow (mean deposition velocity of 0.024?±?0.014 cm s?1) accounting for a diurnally averaged loss rate that was ??30% as large as the net photochemical destruction. From the measurement of deposition velocity an ozone reactivity of ??50 s?1 in seawater is inferred. Due to the unprecedented measurement accuracy of the dynamical budget terms, unobserved photochemistry was able to be deduced, leading to the conclusion that 3.9?±?3.0 ppt (parts per trillion by volume) of NO is present on average in the daytime tropical marine boundary layer, broadly consistent with several previous studies in similar environments. It is estimated, however, that each ppt of BrO hypothetically present would counter each ppt of NO above the requisite 3.9 ppt needed for budget closure. The long-term budget of ozone is further analyzed in the buffer layer, between the boundary layer and free troposphere, and used to derive an entrainment velocity across the trade wind inversion of 0.51 ± 0.38 cm s?1.  相似文献   

7.
Black carbon aerosols plays an important role in the earth's radiative balance and little is known of their concentrations, distributions, source strength, and especially the aerosol chemistry of the developing world. The present study addresses the impact of back carbon aerosols on different atmospheric species like CO and tropospheric ozone over an urban environment, namely Hyderabad, India. Ozone concentration varies from 14 to 63 ppbv over the study area. Diurnal variations of ozone suggest that ozone concentration starts increasing gradually after sunrise, attaining a maximum value by evening time and decreasing gradually thereafter. Black carbon (BC) aerosol mass concentrations varies from 1471 to 11,175 ng m−3. The diurnal variations of BC suggest that the concentrations are increased by a factor of 2 during morning (06:00–09:00 h) and evening hours (18:00 to 22:00 h) compared to afternoon hours. Positive correlation has been observed between BC and CO (r2=0.74) with an average slope of 6.4×10−3 g BC/g CO. The slope between black carbon aerosol mass concentration and tropospheric ozone suggests that every 1 μg m−3 increase in black carbon aerosol mass concentration causes a 3.5 μg m−3 reduction in tropospheric ozone. The results have been discussed in detail in the paper.  相似文献   

8.
Estimates of tropospheric ozone in the East Asian region were obtained using the TOMS and SAGE II satellite data sets through the application of residual analysis on a regional scale. The resulting tropospheric residual ozone shows seasonal variability with highest values in spring and summer. Latitudinal variations give indications of possible input to the tropospheric ozone column from anthropogenic activity. A strong correlation between residual and TOMS total ozone data during summer time suggests a significant level of photochemical ozone production in this region during this period. Comparisons are made with surface ozone measurements from remotely located sites in Japan and show a similar overall pattern.  相似文献   

9.
我国对流层大气臭氧的数值模拟   总被引：7，自引：2，他引：7  
何东阳  黄美元 《大气科学》1993,17(6):741-749
本文建立了一个用于对流层大气臭氧模拟的三维欧拉模式,针对影响臭氧光化学转化的各种因素及我国城市光化学污染的特点,模式中简化了光化学项的计算。根据实际观测资料,提出了模拟云雾对臭氧影响的参数化方法,并确定了云雾作用系数,通过模式的数值模拟,得出了我国对流层大气臭氧,特别是近地面层大气臭氧的分布状况、我国城市光化学污染的分布特征以及它们的季节变化规律.  相似文献   

10.
Temporal-spatial variations in tropospheric ozone concentrations over East Asia in the period from 1 January 2000 to 31 December 2004 were simulated by using the Models-3 Community Multi-scale Air Quality (CMAQ) modeling system with meteorological fields calculated by the Regional Atmospheric Modeling System (RAMS). The simulated concentrations of ozone and carbon monoxide were compared with ground level observations at two remote sites, Ryori (39.03°N, 141.82°E) and Yonagunijima (24.47°N, 123.02°E). The co...  相似文献   

11.
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   

12.
Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.  相似文献   

13.
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   

14.
Summary The application of principal components and cluster analysis to vertical ozone concentration profiles in Tsukuba, Japan, has been explored. Average monthly profiles and profiles of the ratio between standard deviation and the absolute ozone concentration (SDPR) of 1 km data were calculated from the original ozone concentration data. Mean (first) and gradient (second) components explained more than 80% of the variation in both the 0–6 km tropospheric and 11–20 km troposphere–stratosphere (interspheric) layers. The principal components analysis not only reproduced the expected inverse relationship between mean ozone concentration and tropopause height (r 2 = 0.41) and that in the tropospheric layer this is larger in spring and summer, but also yielded new information as follows. The larger gradient component score in summer for the interspheric layer points to the seasonal variation of the troposphere–stratosphere exchange. The minimum SDPR was at about 3 km in the tropospheric layer and the maximum was at about 17 km in the interspheric layer. The tropospheric SDPR mean component score was larger in summer, possibly reflecting the mixing of Pacific maritime air masses with urban air masses. The cluster analysis of the monthly ozone profiles for the 1970s and 2000s revealed different patterns for winter and summer. The month of May was part of the winter pattern in the 1970s but part of the summer pattern during the 2000s. This statistically detected change likely reflects the influence of global warming. Thus, these two statistical analysis techniques can be powerful tools for identifying features of ozone concentration profiles. Authors’ addresses: S. Yonemura, S. Kawashima, S. Inoue, National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-0031, Japan; H. Matsueda, Y. Sawa, Meteorological Research Institute, 1-1 Nagamine, Tsukuba, Ibaraki 305-0052, Japan; H. Tanimoto, National Institute for Environmental Studies, 16-2 Onogawa, Tsukuba, Ibaraki 305-8506, Japan.  相似文献   

15.
Scientists have long debated the relative importance of tropospheric photochemical production versus stratospheric influx as causes of the springtime tropospheric ozone maximum over northern mid-latitudes. This paper investigates whether or not stratospheric intrusion and photochemistry play a significant role in the springtime ozone maximum over Northeast Asia,where ozone measurements are sparse.We examine how tropospheric ozone seasonalities over Naha(26°N,128°E),Kagoshima(31°N,131°E),and Pohang(36°N,129°E),which are located on the same meridional line,are related to the timing and location of the jet stream.The ozone seasonality shows a gradual increase from January to the maximum ozone month,which corresponds to April at Naha,May at Kagoshima,and June at Pohang.In order to examine the occurrence of stratospheric intrusion,we analyze a correlation between jet stream activity and tropospheric ozone seasonality.From these analyses,we did not find any favorable evidence supporting the hypothesis that the springtime enhancement may result from stratospheric intrusion.According to trajectory analysis for vertical and horizontal origins of the airmass,a gradual increasing tendency in ozone amounts from January until the onset of monsoon was similar to the increasing ozone formation tendency from winter to spring over mainland China,which has been observed during the build-up of tropospheric ozone over Central Europe in the winter-spring transition period due to photochemistry.Overall,the analyses suggest that photochemistry is the most important contributor to observed ozone seasonality over Northeast Asia.  相似文献   

16.
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17.
This study estimated the largely unstudied downward transport and modification of tropospheric ozone associated with tropical moist convection using a coupled meteorology-chemistry model. High-resolution cloud resolving model simulations were conducted for deep moist convection events over West Africa during August 2006 to estimate vertical transport of ozone due to convection. Model simulations realistically reproduced the characteristics of deep convection as revealed by the estimated spatial distribution of temperature, moisture, cloud reflectivity, and vertical profiles of temperature and moisture. Also, results indicated that vertical transport reduced ozone by 50% (50 parts per billion by volume, ppbv) in the upper atmosphere (12–15 km) and enhanced ozone by 39% (10 ppbv) in the lower atmosphere (<2 km). Field observations confirmed model results and indicated that surface ozone levels abruptly increased by 10–30 ppbv in the area impacted by convection due to transport by downdrafts from the upper troposphere. Once in the lower troposphere, the lifetime of ozone decreased due to enhanced dry deposition and chemical sinks. Ozone removal via dry deposition increased by 100% compared to non-convective conditions. The redistribution of tropospheric ozone substantially changed hydroxyl radical formation in the continental tropical boundary layer. Therefore, an important conclusion of this study is that the redistribution of tropospheric ozone, due to deep convection in non-polluted tropical regions, can simultaneously reduce the atmospheric loading of ozone and substantially impact the oxidation capacity of the lower atmosphere via the enhanced formation of hydroxyl radicals.  相似文献   

18.
Modelling of near-surface ozone over South Asia   总被引：2，自引：1，他引：1  
Hourly, three-dimensional, fields of tropospheric ozone have been produced for 12 consecutive months on a domain covering South Asia, using the regional Eulerian off-line chemistry transport model MATCH. The results were compared with background observations to investigate diurnal and seasonal variations of near-surface ozone in the region. MATCH reproduced the seasonality of near-surface ozone at most locations in the area. However, the current, and previous, studies indicate that the model consequently overestimate night-time concentrations, while it occasionally underestimates the day-time, near-surface, ozone concentrations. The lowest monthly-mean concentrations of near-surface ozone are typically experienced in June–September, coincident with the rainy season in most areas. The seasonality is not identical across the domain; some locations have a completely different trend. Large areas in Northern India and Nepal show a secondary minimum during the cold winter season (December–January). High concentrations of near-surface ozone are found over the oceans, close to the Indian subcontinent, due to the less efficient dry deposition to water surfaces; over parts of Tibet due to influence of free tropospheric air and little deposition to snow covered surfaces; and along the Gangetic valley due to the large emissions of precursors in this region. Monthly-mean ozone concentrations in the densely populated northern India range from 30–45 ppb(v). The model results were also used to produce maps of AOT40. The results point towards similar levels of AOT40 in India as in Europe: large areas of India show 3-month AOT40 values above 3 ppm(v) hours.
Magnuz EngardtEmail:
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19.
The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.  相似文献   

20.
Several studies have shown that in qualitative terms VOCs can be ranked in terms of their importance to ozone formation in Europe, using a so-called photochemical ozone creation potential (POCP). However, all studies showed significant variability in the quantitative POCP values assigned to each VOC species. In this paper, we make use of a complex photochemical oxidant model to quantify how the reaction time-scales of emitted VOC and their reaction products vary with geographical location and time of year. The model is used to evaluate monthly POCP values for 9 hydrocarbon and oxygenated VOC compounds for a cross-section across Europe. Calculations are presented to illustrate the gradients in POCP values of one species,n-butane, across the whole of Europe for April and June 1989. We discuss some of the factors responsible for these variations.  相似文献   

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