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1.
Atmospheric hydroxyl (OH), hydroperoxy (HO2), total peroxy (HO2 and organic peroxy radicals, RO2) mixing ratios and OH reactivity (first order OH loss rate) were measured at a rural site in central Pennsylvania during May and June 2002. OH and HO2 mixing ratios were measured with laser induced fluorescence (LIF); HO2 + RO2 mixing ratios were measured with chemical ionization mass spectrometry (CIMS). The daytime maximum mixing ratios were up to 0.6 parts per trillion by volume (pptv) for OH, 30 pptv for HO2, and 45 pptv for HO2 + RO2. A parameterized RACM (Regional Atmospheric Chemistry Mechanism) box model was used to predict steady state OH, HO2 and HO2 + RO2 concentrations by constraining the model to the measured OH reactivity and previously measured volatile organic compound (VOC) distributions. The averaged model calculations are generally in good agreement with the observations. For OH, the model matched the observations for day and night, with an average observed-to-modeled ratio of 0.80. In previous studies such as PROPHET98, nighttime NO was near 0 pptv and observed nighttime OH was significantly larger than modeled OH. In this study, nighttime observed and modeled OH agree to within measurement and model uncertainties because the main source of the nighttime OH was the reaction HO2 + NO → OH + NO2, with the NO being continually emitted from the surrounding fertilized corn field. The observed-to-modeled ratio for HO2 is 1.0 on average, although daytime HO2 is underpredicted by a factor of 1.2 and nighttime HO2 is over-predicted by a factor of ∼2. The average measured and modeled HO2 + RO2 agree well during daytime, but the modeled value is about twice the measured value during nighttime. While measured HO2 + RO2 values agree with modeled values for NO mixing ratios less than a few parts per billion by volume (ppbv), it increases substantially above the expected value for NO greater than a few ppbv. This observation of the higher-than-expected HO2 + RO2 with the CIMS technique confirms the observed increase of HO2 above expected values at higher NO mixing ratios in HO2 measurements with the LIF technique. The maximum instantaneous O3 production rate calculated from HO2 and RO2 reactions with NO was as high as 10–15 ppb h−1 at midday; the total daily O3 production varied from 13 to 113 ppbv d−1 and was 48 ppbv d−1 on average during this campaign.  相似文献   

2.
Observations of the Nitrate Radical in the Marine Boundary Layer   总被引：3，自引：0，他引：3  
A study of the nitrate radical (NO3) has been conducted through a series of campaigns held at the Weybourne Atmospheric Observatory, located on the coast of north Norfolk, England. The NO3 concentration was measured in the lower boundary layer by the technique of differential optical absorption spectroscopy (DOAS). Although the set of observations is limited, seasonal patterns are apparent. In winter, the NO3 concentration in semi-polluted continental air masses was found to be of the order of 10 ppt, with an average turnover lifetime of 2.4 minutes. During summer in clean northerly air flows, the concentration was about 6 ppt with a lifetime of 7.2 minutes. The major loss mechanisms for the radical were investigated in some detail by employing a chemical box model, constrained by a suite of ancillary measurements. The model indicates that during the semi-polluted conditions experienced in winter, the major loss of NO3 occurred indirectly through reactions of N2O5, either in the gas-phase with H2O, or through uptake on aerosols. The most important direct loss was via reactions of NO3 with a number of unsaturated nonmethane hydrocarbons. The cleaner air masses observed during the summer were of marine origin and contained elevated concentrations of dimethyl sulfide (DMS), which provided the major loss route for NO3. The box model was then used to investigate the conditions in the remote marine boundary layer under which DMS will be oxidised more rapidly at night (by NO3) than during the day (by OH). This should occur if the concentration of NO2 is more than about 60% that of DMS.  相似文献   

3.
Measurements of surface ozone (O3), nitric oxide (NO), nitrogen dioxide (NO2), oxides of nitrogen (NOx=NO+NO2) and meteorological parameters have been made at Agra (North Central India, 27°10??N, 78°05??E) in post monsoon and winter season. The diurnal variation in O3 concentration shows daytime in situ photochemical production with diurnal maximum in noon hours ranging from 51 to 54 ppb in post monsoon and from 76 to 82 ppb in winter, while minimum (16?C24 ppb) during nighttime and early morning hours. Average 8-h O3 concentration varied from 12.4 to 83.9 ppb. The relationship between meteorological parameters (solar radiation intensity, temperature, relative humidity, wind speed and wind direction) and surface O3 variability was studied using principal component analysis (PCA), multiple linear regression (MLR) and correlation analysis (CA). PCA and MLR of daily mean O3 concentrations on meteorological parameters explain up to 80 % of day to day ozone variability. Correlation with meteorology is strongly emphasized on days having strong solar radiation intensity and longer sunshine time.  相似文献   

4.
利用统计方法和数值模拟对2008年4月18日-7月28日和2009年5月19日-8月20日在黄山光明顶的两次外场观测中臭氧（O3）数据进行了分析,讨论了中国华东高海拔地区O3的质量浓度特征和来源。结果表明,5、6和7月的月平均质量浓度分别为107．73、101．93和68．02μg·m^-1,其中5月和6月的月平均质量浓度相对于国内其他本底站（除上甸子外）以及南极地区高出25～60Iμg·m^-1,7月与其他地区质量浓度相差较少。该地区的0,质量浓度相对于其他地区整体上维持在一个较高的水平,但高质量浓度超标事件发生的次数很少,只占总观测时间的3．9％。质量浓度EI最大值多出现在夜间21时一次日06时（北京时间,下同）,呈多峰分布,并且变化幅度很小,在15—20μg·m^-1,通过利用WRF（Weather Research and Forecasting）模式模拟当地上空对流层顶高度和晴空湍流等要素的变化发现,O3质量浓度和对流层顶折叠现象有关。不同天气条件下,其质量浓度在晴天最高,雨天最低,雾天和阴天在二者之间。臭氧质量浓度与温度、相对湿度和其他污染气体（CO、N0和NO3）浓度之间有很强的负相关,而与风速相关性相对较弱;5月北面来风占主导,各风向所对应的O3质量浓度分布较均匀,而6月和7月西南风占主导,北面来向的风对应的质量浓度要高于南面来向。在利用KZ过滤器将O3原始数据分解成不同组份后,发现当地O3质量浓度整体上受低频组份（CBL组份）的控制,其余各高频组份（CSY、CDU和CID组份）只是会使其质量浓度在基准线附近波动。随后对发生在2009年5月28—31日和6月12—15日期间的两次0,质量浓度超标事件中CSY、CDU和CID对基线的贡献做了定量分析。  相似文献   

5.
Observations of the concentration of several nitrogen containing compounds at five rural Scandinavian sites during March–June 1993 are reported. Total nitrate (NO 3 - + HNO3) and total ammonium (NH 4 + + NH3) were measured by denuder and filter pack. In general the methods agree well. At all sites the particulate fraction dominated, with the largest fraction of NO 3 - and the lowest of NH 4 + at the sites which were closest to the emission sources. The fraction of NO 3 - of total nitrate increased with increasing NO2 concentrations, indicating that the nighttime conversion of NO2 to NO 3 - is an important route of formation for NO 3 - . A positive correlation was found between HNO3 and O3 in June at all sites, while no correlation was found early in the spring. Model calculations were made with a lagrangian boundary layer photooxidant model for the whole period, and compared to the measured concentrations. The calculated ratio between mean observed and modelled daily maximum concentrations of ozone over the measurement period were within +/–10% at all sites. The models ability to describe the daily ozone maximum concentration was satisfactory with an average deviation of 19–22% from the observed concentrations. HNO3 was underestimated by over 50% at all sites except the one closest to the emission sources. The correlation between modelled and observed concentrations was generally best for the sites with shortest transport distance from the sources of emission.  相似文献   

6.
利用2004～2006年杭州主城区环境空气监测资料,研究了O_3、NO_2和CO浓度的分布特征和时间变化规律,结果表明,杭州主城区3年的O_3、NO_2、CO的年均浓度都不大,分别为40、60、1400μg·m~(-3).四季中O_3、NO_2和CO浓度相差较大,O_3是夏季高冬季低,NO_2和CO则是秋季较高,夏季较低.O_3、NO_2和CO浓度日变化也很明显,其中O_3是单峰形态,NO_2和CO为双峰形态.不同天气条件下O_3与烃类的关系研究表明,晴天时烃类浓度减少,O_3浓度明显增加;阴天时O_3浓度较低,烃类浓度较高,它们的变化不大.白天和夜晚不同风速时O_3、C_2-C_(12)的浓度变化不同,白天风速增大时C_2-C_(12)浓度减小,O_3浓度增加;晚上无此变化.  相似文献   

7.
The Weather Research and Forecasting/Chemistry model(WRF-Chem) was updated by including photoexcited nitrogen dioxide(NO2) molecules,heterogeneous reactions on aerosol surfaces,and direct emissions of nitrous acid(HONO) in the Carbon-Bond Mechanism Z(CBM-Z).Five simulations were conducted to assess the effects of each new component and the three additional HONO sources on concentrations of major chemical components.We calculated percentage changes of major aerosol components and concentration ratios of gas NO y(NOyg) to NO y and particulate nitrates(NO-3) to NO y due to the three additional HONO sources in the North China Plain in August of 2007.Our results indicate that when the three additional HONO sources are included,WRF-Chem can reasonably reproduce the HONO observations.Heterogeneous reactions on aerosol surfaces are a key contributor to concentrations of HONO,nitrates(NO 3),ammonium(NH + 4),and PM 2.5(concentration of particulate matter of 2.5 μm in the ambient air) across the North China Plain.The three additional HONO sources produced a～5%-20% increase in monthly mean daytime concentration ratios of NO-3 /NO y,a ～15%-52% increase in maximum hourly mean concentration ratios of NO-3 /NO y,and a ～10%-50% increase in monthly mean concentrations of NO-3 and NH+4 across large areas of the North China Plain.For the Bohai Bay,the largest hourly increases of NO-3 exceeded 90%,of NH+4 exceeded 80%,and of PM 2.5 exceeded 40%,due to the three additional HONO sources.This implies that the three additional HONO sources can aggravate regional air pollution,further impair visibility,and enhance the incidence of haze in some industrialized regions with high emissions of NO x and particulate matter under favorable meteorological conditions.  相似文献   

8.
Eddy correlation measurements of NO vertical flux were made periodically from October 1983 through June 1984 at a height of eight meters above grass in northeastern Illinois, U.S.A. From 207 data points, each representing a 25 min average, 19 daytime cases and 8 nighttime cases were selected on the basis of steady, nonadvective atmospheric conditions. Each case was represented by a set of data constituting a 3 to 5 hr average. Concentrations of O3, NO, and NO y (from which NO2 was inferred) and local atmospheric and surface conditions also were measured, to provide the information necessary to assess the relative importance of surface deposition, surface emission, and air chemistry on the observed NO flux. On the basis of a linear regression analysis applied with independent variables representing physical, chemical, and biological processes, surface uptake of NO was very small for data primarily collected in the daytime during spring, and measured deposition velocities at a height of 8 m were very small, much smaller than expected for NO2. For the same time period, the surface emission rates of elemental nitrogen in NO were in the range of 1.4 to 4.2 ng m-2 s-1 for moist, unsaturated soils at temperatures near 15° C. These emissions were partially masked in the measured fluxes by rapid in-air chemical reactions involving O3 and NO2. The effects of rapid in-air chemical reactions involving O3 were to decrease the (upward) flux of NO with height. While the information collected at night was too limited to strongly support hypotheses concerning emissions and deposition, a pathway for NO production by reactions involving NO3 and related compounds was indicated. For daytime conditions, this production pathway is not evident, probably because of the relatively strong effects of photochemical reactions involving NO, NO2, and O3.Formerly with the Chemical Technology Division of Argonne National Laboratory and currently affiliated with Bio-Rad Laboratories, Digilab Division, Minneapolis, MN, U.S.A.  相似文献   

9.
Spatio-temporal distribution characteristics and variation trends of tropospheric NO_2 in Pearl River Delta(PRD) urban group and its adjacent areas were analyze from 2005 to 2013 based on remote sensing data from ozone monitoring instrument(OMI) satellite, and further explored the impact of human activities on NO_2. Compared with the ground observation data, the OMI NO_2 remote sensing data displayed high reliability. Due to active industrial production, high car ownership, great energy and power consumption, the average tropospheric NO_2concentration(7.4×1015molec/cm2) of PRD region is about 3 times of the adjacent areas. At the same time, the regional high pollution NO_2 in PRD region as a whole, the urban group effect is remarkable. Sinusoidal model can well fit the periodic variation of the NO_2 in PRD and adjacent areas. NO_2 concentration was highest in winter while lowest in summer. The concentration of NO_2 in PRD region is decreasing in recent 9 years, which has a significantly negative correlation with the second industry output and car ownership. This suggests that the nitrogen oxide emissions governance in PRD region had achieved initial results. The concentration of NO_2 increased significantly in the eastern and northern Guangdong Province, there are good positive correlations with the second industrial outputs and car ownerships, it is thus clear that industrial emissions and automobile exhausts are important sources of NO_2 in these regions. The concentration of NO_2 in western Guangdong area is stable.  相似文献   

10.
将INTEX-B排放源应用到空气质量模型Model3-CMAQ中,对中国地区对流层NO2的浓度分布进行了数值模拟,并与OMI卫星对流层NO2资料进行了对比和验证。结果表明：将INTEX-B排放源应用到Model3-CMAQ模式,模拟的NO2浓度在中国地区的分布、季节变化规律与卫星资料所得结果一致。敏感性试验表明,工业及电厂排放对NO2的浓度贡献最大,而交通排放的贡献相对较小,两种排放均主要集中在京津、长江三角洲等经济发达地区。  相似文献   

11.
南京北郊冬季大气SO2、NO2和O3的变化特征   总被引：1，自引：0，他引：1  
利用差分吸收光谱仪DOAS（differential optical absorption spectroscopy）,对2007年11月—2008年1月南京北郊大气SO2、NO2和O3进行了观测。结合Parsivel降水粒子谱仪和自动气象站的资料,对冬季大气污染气体的浓度变化规律及降水和风速风向对其的影响进行了分析。结果表明,南京北郊大气SO2浓度较高,呈明显双峰特征,分别在12时（北京时,下同）和00时达最大,受附近排放源的影响最大,东风及南风时比静风时SO2浓度更高。降水对SO2湿清除效果明显,清除系数平均为0.168 h-1。NO2气体呈明显单峰特征,在18时达最高值。南京北郊是NO2源区之一,主要受附近高速公路汽车尾气排放源的影响。静风时NO2浓度最高。O3浓度受NO2的影响较明显。O3日变化呈单峰特征,在15时达最大值,静风时O3浓度最低。降水对O3的间接影响较明显,在降水时,白天由于太阳辐射较弱,O3浓度降低;夜晚NO浓度较低,使得O3浓度升高。  相似文献   

12.
四川盆地是我国夜雨发生频次最高的地区，夜间暴雨是夜雨中可致灾并加剧防范难度的一类特殊气象灾害，但以往对四川山地夜间暴雨精细特性的相关研究较少。利用四川省2010—2019年2 165个国家及区域气象站逐小时降水资料，分区统计了四川暖季（5—9月）暴雨日夜间降水占日降水量的比例、夜间暴雨频次和夜间平均暴雨强度的基本特征，并通过趋势分析和地理加权回归等统计方法，分析了其空间分布及其与海拔高度的关系，获得以下结果：（1）四川暴雨日夜间降水占日降水量比例呈现自南向北递减的趋势，以海拔2 800 m为分界，表现为随海拔高度升高呈先增大、后减小的垂直分布特征，川西南山地与其他山地区域整体上升的变化趋势明显不同。（2）夜间暴雨频次较多的测站沿川西与川西南山地陡峭地形呈线性分布，夜间暴雨频次随海拔高度升高总体呈现减小的特征，川西山地和川西南山地的频次最大值分别出现在海拔800 m和500 m。（3）四川夜间平均暴雨强度整体随海拔的升高而减小，大值区主要位于川西山地和川东北山地，海拔700 m高度处的峰值强度主要由川西山地贡献。（4）川西山地夜间暴雨特征呈次数较多且每次强度大，川西南山地夜间暴雨为次数多但单次降水量较小，而川东北夜间暴雨的强度较大但次数较少。以上结果有助于深化对山地夜间暴雨精细特征的认识。  相似文献   

13.
The air quality model CMAQ-MADRID （Community Multiscale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization and Dissolution） was employed to simulate summer O3 formation in Beijing China, in order to explore the impacts of four heterogeneous reactions on O3 formation in an urban area. The results showed that the impacts were obvious and exhibited the characteristics of a typical response of a VOC-limited regime in the urban area. For the four heterogeneous reactions considered, the NO2 and HO2 heterogeneous reactions have the most severe impacts on O3 formation. During the O3 formation period, the NO2 heterogeneous reaction increased new radical creation by 30%, raising the atmospheric activity as more NO→NO2 conversion occurred, thus causing the O3 to rise. The increase of O3 peak concentration reached a maximum value of 67 ppb in the urban area. In the morning hours, high NO titration reduced the effect of the photolysis of HONO, which was produced heterogeneously at night in the surface layer. The NO2 heterogeneous reaction in the daytime is likely one of the major reasons causing the O3 increase in the Beijing urban area. The HO2 heterogeneous reaction accelerated radical termination, resulting in a decrease of the radical concentration by 44% at the most. O3 peak concentration decreased by a maximum amount of 24 ppb in the urban area. The simulation results were improved when the heterogeneous reactions were included, with the O3 and HONO model results close to the observations.  相似文献   

14.
The amounts of SOA and reactive oxygen species (ROS) formed by the reaction of α-pinene with ozone (O3) in the presence of nitric oxide (NO) were studied by varying the ratio of O3 to NO in a chamber under conditions that simulate the indoor environment. The particle mass was measured using a tapered element oscillating microbalance (TEOM) and a scanning mobility particle sizer (SMPS) was used to obtain particle volume distributions. The concentrations of particle-bound reactive species (ROS) were quantitatively determined from collected filters by the measuring the oxidation of dichlorofluorescin (DCFH) to a fluorescent product. The measured fluorescent intensities were converted to equivalent H2O2 concentrations. Three sets of experiments using different concentration ratios of NO/O3 were conducted. Measured steady-state, particle-bound ROS concentrations ranged from 0.58 to 6.78 nmol/m3 of H2O2. The SOA yields were examined using Odum’s SOA yield model that relates the mass of SOA formed to the mass of hydrocarbon consumed. For the condition where NO and O3 were in a concentration ratio of 0.5, the SOA yield was the highest with 22 % of α-pinene converted to SOA. Under these experimental conditions, the highest concentration of nitrate radical in these experiments would have been produced.  相似文献   

15.
利用ＬＬＡ－Ｃ光化学反应机制,在ＮＯＸ保持高值不变时,模拟分布范围很广的８种初始［ＮＭＨＣ］／［ＮＯｘ］（１０９／１０９）（１．０、３．０、７．１、１４．３、２８．６、５７．２、１００．０、２００．０）条件下臭氧体积分数的变化。模拟结果表明,当［ＮＭＨＣ］／［ＮＯｘ］≥１５．０时,臭氧生成量对ＮＭＨＣ的改变不大敏感而主要依赖于ＮＯｘ的大小。但是,当非甲烷烃与氮氧化物的比北较低（＜７．０）时,臭氧生成量紧密地依赖于非甲烷烃体积分数。进一步的验证工作还有待于加强。  相似文献   

16.
The chemistry version of the Weather Research and Forecasting model (WRF/Chem) was coupled with the anthropogenic emission inventory of David Streets to investigate the impacts of secondary aerosols on a persistent fog event from 25 to 26 October 2007, in Northern China. The spatial distribution of the simulated fog is consistent with satellite observations, and the time-height distributions of the simulated boundary layer where the fog formed are also in good agreement with these observations. The sensitivity studies show that the secondary aerosols of SO 4 , NO 3 , and NH 4 formed from gaseous precursors of SO 2 , NO x , and NH 3 had substantial impacts on the formation processes and microphysical structure of the fog event. The decrease of the secondary aerosols obviously reduced the liquid water path and column droplet number concentration of the fog below the 1-km layer, and the corresponding area-averaged liquid water path and droplet number concentration of the fog decreased by 43% and 79%, respectively. The concentrations of NO x and NO 3 were found to be extremely high in this case. The concentration of interstitial aerosol NO 3 was much higher than the SO 4 and NH 4 , but the concentration of SO 4 was highest in the cloud-borne aerosols. The average activation ratios for SO 4 , NO 3 , and NH 4 were 34%, 31%, and 30%, respectively, and the maximum ratios reached 62%, 86%, and 55% during the fog episode.  相似文献   

17.
Using the Differential Absorption Lidar (DIAL) technique, two types of approaches, namely, reflection from retroreflector/topographic target and backscatter from atmosphere, are available for studying remotely the atmos-pheric NO2 concentration. The Argon ion lidar system at the Indian Institute of Tropical Meteorology (IITM), Pune, India has been used for the measurements by following both the path-averaged and range-resolved ap-proaches. For the former, a topographic target (hill) is used for determining path-averaged surface concentration. In the latter, spectral properties of atmospheric attenuation is used for making range-resolved measurements in the sur-face layer. The results of the observations collected by following both approaches are presented. The average surface NO2 concentration was found to vary between 0.01 and 0.105 ppm and the range-resolved measurements exhibited higher values suggesting treatment of the lidar data for scattering and extinction effects due to atmospheric aerosols and air molecules, and atmospheric turbulence. Certain modifications that arc suggested to the experimental set-up, data acquisition and analysis to improve the measurements are briefly described.  相似文献   

18.
区域性光化学模式与LLA-C机制的模拟性能比较   总被引：1，自引：0，他引：1  
以 Ｌ Ｌ Ａ－ Ｃ 机制为基准,在［ Ｎ Ｍ Ｈ Ｃ］／［ Ｎ Ｏ＃ － ｘ］ 比率分别为１７９ 、７１４ 、２８６ 条件下测试了区域性光化学模式（ Ｒ Ｏ Ｓ） 的模拟性能。结果表明 Ｒ Ｏ Ｓ 模式在上述三种初值条件下均能从总体趋势上给出与 Ｌ Ｌ Ａ － Ｃ 机制相似的结果, 但只有当非甲烷烃浓度较高（［ Ｎ Ｍ Ｈ Ｃ］／［ Ｎ Ｏｘ］ ＞ １２） 时 Ｒ Ｏ Ｓ 模式模拟值与 Ｌ Ｌ Ａ－ Ｃ 机制预测值比较接近。在这种条件下, Ｒ Ｏ Ｓ 模型对 Ｏ Ｈ 的预测值有待改进。我国大气中相当高的［ Ｎ Ｍ Ｈ Ｃ］／［ Ｎ Ｏｘ］ 比率说明 Ｒ Ｏ Ｓ 模式用于全国范围内的空气质量趋势模拟是可行的。  相似文献   

19.
To investigate the impacts of the diurnal cycle on tropical cyclones （TCs）,a set of idealized simulations were conducted by specifying different radiation （i.e.,nighttime-only,daytime-only,full diurnal cycle）.It was found that,for an initially weak storm,it developed faster during nighttime than daytime.The impacts of radiation were not only on TC intensification,but also on TC structure and size.The nighttime storm tended to have a larger size than its daytime counterparts.During nighttime,the radiative cooling steepened the lapse rate and thus reduced the static stability in cloudy regions,enhancing convection.Diabatic heating associated with outer convection induced boundary layer inflows,which led to outward expansion of tangential winds and thus increased the storm size.  相似文献   

20.
The applicability of the tungsten oxide denuder tube technique for the measurement of nitric acid in the rural troposphere was investigated. The technique is based on selective chemisorption of HNO3 from the gas stream, thermal desorption, conversion to NO, and analysis by NO–O3 chemiluminescence. Ammonia, which is also collected and desorbed as NH3 and NO, was separated from the HNO3-derived NO by linear temperature-programed thermal desorption. Possible interferences by NO2, HCN, PAN, and n-propyl nitrate (NPN) were tested and found to be significant under conditions found in the lower troposphere. Simultaneous ambient measurements of HNO3 were made with the tungsten oxide denuder tube and nylon filter methods at a rural site in the Colorado mountains (Niwot Ridge, CO). Nitric acid levels measured by the tungsten oxide denuder tube averaged a factor of 3 higher than levels measured by the nylon filter technique. Tests involving the placement of nylon materials in front of the tungsten oxide denuder tube show that there are species, as yet unidentified, present in the atmosphere that interfere with the measurement of HNO3 by the tungsten oxide technique.  相似文献   

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