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1.
为了进一步了解青藏高原闪电的产生氮氧化物（LNOx）经由光化学反应对O3浓度变化及夏季O3低谷形成的可能影响,本文利用2005~2013年由OMI卫星得到的对流层NO2垂直浓度柱（NO2 VCD）、O3总浓度柱（TOC）和O3廓线以及星载光学瞬变探测器OTD和闪电成像仪LIS获取的总闪电数资料,对青藏高原和同纬度长江中下游地区的TOC和NO2 VCD月均值时空分布特征、闪电与NO2 VCD的相关性和O3的垂直分布特征及其与LNOx的关系进行了对比分析。结果表明,青藏高原的O3低谷主要出现在夏季和秋季,其TOC值比同纬度长江中下游地区低约10~15 DU（Dobson unit）。青藏高原NO2VCD总体较小,表现为夏高冬低的分布特征。青藏高原夏季O3浓度受南亚高压的影响总体呈减小趋势,但因强雷暴天气导致对流层中上部LNOx浓度升高,并随强上升气流向对流层顶输送,同时通过光化学反应使O3浓度增加,缩小了青藏高原和同纬度地区的O3浓度差,减缓了O3总浓度的下降,抑制了夏季O3低谷的进一步深化。 相似文献
2.
为了解闪电对对流层上部微量气体的贡献,利用全球水资源和气候中心(GHRC)提供的1995年4月—2006年6月的闪电卫星格点资料,以及高层大气研究卫星(UARS)上的卤素掩星试验(HALOE)1991年10月—2005年11月的观测资料,分析了全球闪电与对流层上部NO和O3体积分数的时空分布特征及其相关性。结果表明:全球闪电12、1、2月集中在南半球,6—8月集中在北半球,全球闪电的季节分布与NO、O3类似;NO体积分数在350 h Pa附近达到最大,该高度的南半球NO体积分数变化范围为7×10-12~11×10-12、北半球为3×10-12~17×10-12;450~300 h Pa,北半球夏季O3体积分数呈明显增加趋势,且同一高度上夏季的值比年平均值大25%左右,南半球夏季O3体积分数高于冬季,但差异并不大。结论进一步证明了闪电与对流层上部NO及O3的密切关系,也为研究全球气候变化提供有力证据。 相似文献
3.
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
4.
利用GOME (Global Ozone Monitoring Experiment, 全球臭氧监测实验) 1996年1月—2002年12月NO2对流层柱浓度月平均卫星遥感资料以及根据北京市2001年1月1日—2002年12月31日NO2污染指数数据计算出的地面NO2日均质量浓度值, 分析了北京市城市大气NO2污染变化的季节变化特征以及年际变化, 并将2001年1月—2002年12月北京上空GOME NO2对流层柱浓度月平均值变化与北京市地面NO2日均质量浓度月平均值变化进行了比较, 结果表明两者随时间的变化趋势具有较好的一致性, 据此可以利用GOME NO2对流层柱浓度月平均卫星遥感资料来分析特定区域大气NO2的季节变化和年际变化。 相似文献
5.
闪电放电过程发出很强的光辐射,促进了光化学反应的进行,加快了NO_x向上的垂直输送,造成对流层上部NO_x的增加。闪电生成氮氧化物(LNO_x)是对流层上部NO_x(NO和NO_2)的主要来源,影响了对流层和平流层大气成分的垂直分布。本文利用2005—2013年TRMM卫星LIS传感器闪电密度和Aura卫星OMI传感器对流层NO_2垂直柱总量遥感观测数据,分析了中国地区对流层NO_2柱总量时空分布特征及其与闪电活动的相关性。发现,青藏高原地区对流层NO_2柱总量与闪电密度变化特征一致,表现为夏季高,冬季低,该地区LNO_x估算值约为339mol/次。基于LNO_x估算值分析中国不同地区LNO_x/NO_x百分比分布特征,发现,青藏高原地区春季和夏季LNO_x/NO_x较高,约为20%~60%,秋季和冬季低于20%;与之相比,NO_x排放较为严重的四川盆地、长江三角洲和珠江三角洲等地区普遍低于20%,中国地区LNO_x/NO_x百分比平均值低于10%。由此得出结论,LNO_x是青藏高原地区NO_x的主要排放源,人口密集和工业程度较高的四川盆地、长江三角洲和珠江三角洲地区NO_x主要来自于其它排放源。研究结果揭示了中国地区对流层NO_x柱总量分布特征及其与闪电活动的关系,对于研究闪电过程对于氮氧化物生成量的影响有重要意义。 相似文献
6.
基于2013~2017年重庆北碚区缙云山、蔡家和天生3个环境监测站点日值数据,结合地闪观测数据和相关气象要素资料,采用数理统计方法分析了气象条件与O3浓度的关系,并基于HYSPLIT模型研究了闪电日O3传输路径和潜在源区。结果表明:（1）北碚O3浓度峰值大多出现在7月,低值大多出现在12月,其浓度分布从高到低依次为缙云山、蔡家、天生。（2）对比闪电日与非闪电日大气污染浓度,闪电日NO2、CO平均浓度低于非闪电日,O3则相反,闪电日缙云山O3浓度超标率明显低于蔡家和天生。（3）NO2浓度与地闪频次呈负相关,且天生和蔡家NO2浓度波动大于缙云山,O3浓度与地闪频次呈正相关。（4）夏季闪电日O3气团传输路径主要来自南方。（5）地闪活动发生时O3浓度高于非闪电日,其主要原因是夏季地闪频次较高,电解反应频繁,同时重庆夏季光照时间较长,光化学反应充分,两种反应的叠加效果大于降水清除作用。 相似文献
7.
北半球中层大气中NOx的垂直分布特征 总被引：14，自引：3，他引：14
对UARS卫星1992、1993、1994、1995、1996、1998年夏季的HALOE观测资料分别进行客观分析,把卫星观测资料插值到5°×5°的网格点上.并分别做了30°N和40°N多年平均NO2和NO混合比的垂直剖面分析,各年同纬度不同经度及同经度不同纬度处NO和NO2混合比的垂直分布特征分析.结果表明NO混合比含量在1hPa和l×10-5hPa高度处有两个峰值,0.1hPa处是一个极小值,50hPa到0.3hPa之间NO混合比含量非常稳定,而0.1hPa以上NO含量向上增长.在热层中的NO混合比分布有一定起伏.NO2混合比含量在l00hPa及0.5hPa高度处是极小值,从5hPa到10hPa则为最大值.但l00hPa以下进入对流层后含量急剧增加,往往会超过10-8.在平流层中NO2分布廓线基本吻合,同纬度不同经度极值出现的位置变化不大,但不同纬度极值的位置有一定差异,低纬区极值位置偏高.在中层大气中NOx(NO+NO2)和O3具有非常相似的分布特征,尤其在平流层,它们几乎在同一高度达到极值,说明它们之间有非常密切的联系. 相似文献
8.
为了进一步认识闪电活动与对流层氮氧化物的关系及更准确地估算中国地区闪电产生的氮氧化物(LNOx)总量,选取人口稀疏,工业生产水平较低的青藏高原地区作为研究区域,基于LIS(Lightning Imaging Sensor)和GOME-2(The Global Ozone Monitoring Experiment-2)卫星探测仪资料,分析了青藏高原中部区域2009年1月至2012年2月闪电与对流层NO2垂直浓度(VCD)月均值资料的时空分布特性和相关性。在此基础上,结合Beirle et al.(2004)的LNOx估算方法,估算了中国内陆地区的LNOx产量。结果表明:青藏高原地区对流层NO2与闪电与在年际趋势、空间分布及季节变化上保持很好的一致性,闪电密度与NO2VCD的线性拟合相关系数为0.84,这表明青藏高原地区NOx受人为源影响小,是研究LNOx的理想区域。基于拟合结果,估算得到中国内陆地区LNOx的年均产量为0.15(0.03~0.38)Tg(N)a-1。这一结论进一步缩小了以往研究中中国地区LNOx产量估算的不确定范围,有助于更清楚地认识闪电在中国气候变化中的重要作用。 相似文献
9.
基于2008年9月—2010年9月河北固城生态与农业气象试验站多轴差分吸收光谱仪 (multi-axis differential optical absorption spectroscopy, MAX-DOAS) 获得的太阳散射光谱观测,反演计算该地区NO2对流层柱浓度,分析其季节、日变化特征以及不同来源输送的影响,并与同期NO2地面观测资料和卫星产品进行对比分析。发现固城站NO2对流层柱浓度冬高 (5.14×1016 cm-2) 夏低 (1.28×1016 cm-2);日变化形态在四季均呈现中午低、傍晚高的特征,且冬季最明显。与北京城市区域同期的观测相比,冬季固城站观测值略低,而在春、夏季则偏低较显著。地面风玫瑰图分析显示,来自SW, SSW, NE方向及ENE方向的污染输送对其贡献最大。与地面、卫星NO2观测的对比表明,MAX-DOAS反演的NO2柱浓度与地面观测浓度具有一致的季节和日变化特征,卫星反演的NO2对流层柱浓度产品在华北平原农村地区存在系统性低估。 相似文献
10.
该文介绍了中国科学院大气物理研究所（简称IAP）研制的电化学浓度电池（ECC）型臭氧（O3）探空仪基本性能测试和2013年上半年室外比对观测结果。结果表明:ECC的背景电流（Ibg）在0.1 μA以下或更低;测量O3的响应时间为21~26 s;NO2（SO2）使O3测值偏高（低）;抽气泵低压泵效系数（Cef）在100 hPa高度以下为1.0左右,在该高度以上上升,10 hPa达到1.17±0.10,5 hPa达到1.28±0.16,性能略低于同类进口产品（1.055以下）。国产和进口仪器在气象探空或抽气泵等部件上具有良好兼容性;两者所测O3垂直分布廓线总体一致。IAP O3探空仪O3总量与Brewer光谱仪测值比值为0.9~1.1;Cef和Ibg订正有效降低了IAP O3探空仪在平流层低层与进口仪器测值的差别,这一订正对O3柱浓度在平流层和对流层的贡献分别为约15 DU和4~6 DU;在对流层,IAP O3探空仪测值与进口仪器间的绝对差别稳定且低于0.5 mPa;而平流层受泵效影响较明显。因此,建议IAP O3探空仪提高其Cef的稳定性,参与国际比对测试,国产气象探空平台数据接收处理增加必要的滤波技术以降低平流层探测数据（包括O3）的振荡。 相似文献
11.
Lightning is thought to represent an important source of tropospheric reactive nitrogen species NOx (NO + NO2),but estimates of global production of NOx by lightning varyconsiderably. We evaluate the production of NOx by lightning using a global chemical/transport model, satellite lightning observations, and airborne NOx measurements. Various model calculations are conducted toassess the global NOx production rate of lightning by comparing the model calculations with airborne measurements. The results show that the simulated NOx in the tropical middle and upper troposphere are very sensitiveto the amount and altitude of the lightning NOx used in the model. A global lightning NOx production of 7 Tg N yr–1uniformly distributed in convective clouds or 3.5 Tg N yr–1 distributedin the upper cloud regions produces good agreement between calculated and measured NOx concentrations in the tropics. 相似文献
12.
Nathalie Poisson Maria Kanakidou Paul J. Crutzen 《Journal of Atmospheric Chemistry》2000,36(2):157-230
The impact of natural and anthropogenicnon-methane hydrocarbons (NMHC) on troposphericchemistry is investigated with the global,three-dimensional chemistry-transport model MOGUNTIA.This meteorologically simplified model allows theinclusion of a rather detailed scheme to describeNMHC oxidation chemistry. Comparing model resultscalculated with and without NMHC oxidation chemistryindicates that NMHC oxidation adds 40–60% to surfacecarbon monoxide (CO) levels over the continents andslightly less over the oceans. Free tropospheric COlevels increase by 30–60%. The overall yield of COfrom the NMHC mixture considered is calculated to beabout 0.4 CO per C atom. Organic nitrate formationduring NMHC oxidation, and their transport anddecomposition affect the global distribution of NO
x
and thereby O3 production. The impact of theshort-lived NMHC extends over the entire tropospheredue to the formation of longer-lived intermediateslike CO, and various carbonyl and carboxyl compounds.NMHC oxidation almost doubles the net photochemicalproduction of O3 in the troposphere and leads to20–80% higher O3 concentration inNO
x
-rich boundarylayers, with highest increases over and downwind ofthe industrial and biomass burning regions. Anincrease by 20–30% is calculated for the remotemarine atmosphere. At higher altitudes, smaller, butstill significant increases, in O3 concentrationsbetween 10 and 60% are calculated, maximizing in thetropics. NO from lightning also enhances the netchemical production of O3 by about 30%, leading to asimilar increase in the global mean OH radicalconcentration. NMHC oxidation decreases the OH radicalconcentrations in the continental boundary layer withlarge NMHC emissions by up to 20–60%. In the marineboundary layer (MBL) OH levels can increase in someregions by 10–20% depending on season and NO
x
levels.However, in most of the MBL OH will decrease by10–20% due to the increase in CO levels by NMHCoxidation chemistry. The large decreases especiallyover the continents strongly reduce the markedcontrasts in OHconcentrations between land and oceanwhich are calculated when only the backgroundchemistry is considered. In the middle troposphere, OHconcentrations are reduced by about 15%, although dueto the growth in CO. The overall effect of thesechanges on the tropospheric lifetime of CH4 is a 15%increase from 6.5 to 7.4 years. Biogenic hydrocarbonsdominate the impact of NMHC on global troposphericchemistry. Convection of hydrocarbon oxidationproducts: hydrogen peroxides and carbonyl compounds,especially acetone, is the main source of HO
x
in theupper troposphere. Convective transport and additionof NO from lightning are important for the O3 budgetin the free troposphere. 相似文献
13.
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
14.
R. N. Colvile T. W. Choularton J. N. Cape B. J. Bandy K. N. Bower R. A. Burgess T. J. Davies G. J. Dollard M. W. Gallagher K. J. Hargreaves B. M. R. Jones S. A. Penkett R. L. Storeton-West 《Journal of Atmospheric Chemistry》1996,24(3):211-239
Four case studies are described, from a three-site field experiment in October/November 1991 using the Great Dun Fell flow-through reactor hill cap cloud in rural Northern England. Measurements of total odd-nitrogen nitrogen oxides (NO
y
) made on either side of the hill, before and after the air flowed through the cloud, showed that 10 to 50% of the NO
y
, called NO
z
, was neither NO nor NO2. This NO
z
failed to exhibit a diurnal variation and was often higher after passage through cloud than before. No evidence of conversion of NO
z
to NO3
- in cloud was found. A simple box model of gas-phase chemistry in air before it reached the cloud, including scavenging of NO3 and N2O5 by aerosol of surface area proportional to the NO2 mixing ratio, shows that NO3 and N2O5 may build up in the boundary layer by night only if stable stratification insulates the air from emissions of NO. This may explain the lack of evidence for N2O5 forming NO3
- in cloud under well-mixed conditions in 1991, in contrast with observations under stably stratified conditions during previous experiments when evidence of N2O5 was found. Inside the cloud, some variations in the calculated total atmospheric loading of HNO2 and the cloud liquid water content were related to each other. Also, indications of conversion of NO
x
to NO
z
were found. To explain these observations, scavenging of NO
x
and HNO2 by cloud droplets and/or aqueous-phase oxidation of NO2
- by nitrate radicals are considered. When cloud acidity was being produced by aqueous-phase oxidation of NO
x
or SO2, NO3
- which had entered the cloud as aerosol particles was liberated as HNO3 vapour. When no aqueous-phase production of acidity was occurring, the reverse, conversion of scavenged HNO3 to particulate NO3
-, was observed. 相似文献
15.
Field measurements of NO and NO2 emissions from soils have been performed in Finthen near Mainz (F.R.G.) and in Utrera near Seville (Spain). The applied method employed a flow box coupled with a chemiluminescent NO
x
detector allowing the determination of minimum flux rates of 2 g N m-2 h-1 for NO and 3 g m-2 h-1 for NO2.The NO and NO2 flux rates were found to be strongly dependent on soil surface temperatures and showed strong daily variations with maximum values during the early afternoon and minimum values during the early morning. Between the daily variation patterns of NO and NO2, there was a time lag of about 2 h which seem to be due to the different physico-chemical properties of NO and NO2. The apparent activation energy of NO emission calculated from the Arrhenius equation ranged between 44 and 103 kJ per mole. The NO and NO2 emission rates were positively correlated with soil moisture in the upper soil layer.The measurements carried out in August in Finthen clearly indicate the establishment of NO and NO2 equilibrium mixing ratios which appeared to be on the order of 20 ppbv for NO and 10 ppbv for NO2. The soil acted as a net sink for ambient air NO and NO2 mixing ratios higher than the equilibrium values and a net source for NO and NO2 mixing ratios lower than the equilibrium values. This behaviour as well as the observation of equilibrium mixing ratios clearly indicate that NO and NO2 are formed and destroyed concurrently in the soil.Average flux rates measured on bare unfertilized soils were about 10 g N m-2 h-1 for NO2 and 8 g N m-2 h-1 for NO. The NO and NO2 flux rates were significantly reduced on plant covered soil plots. In some cases, the flux rates of both gases became negative indicating that the vegetation may act as a sink for atmospheric NO and NO2.Application of mineral fertilizers increased the NO and NO2 emission rates. Highest emission rates were observed for urea followed by NH4Cl, NH4NO3 and NaNO3. The fertilizer loss rates ranged from 0.1% for NaNO3 to 5.4% for urea. Vegetation cover substantially reduced the fertilizer loss rate.The total NO
x
emission from soil is estimated to be 11 Tg N yr-1. This figure is an upper limit and includes the emission of 7 Tg N yr-1 from natural unfertilized soils, 2 Tg N yr-1 from fertilized soils as well as 2 Tg N yr-1 from animal excreta. Despite its speculative character, this estimation indicates that NO
x
emission by soil is important for tropospheric chemistry especially in remote areas where the NO
x
production by other sources is comparatively small. 相似文献
16.
A bifurcation phenomenon with relevance to atmospheric chemistry is discussed. The gasphase reactions in the troposphere exhibit two types of temporal evolution which are controlled by the strength of the source,Q, of nitric oxide, NO, via the nonlinear chemical coupling between the hydrogen oxides and nitrogen oxides chemistry. IfQ remains below a threshold value, all short-lived species, including NO, approach steady-state concentrations, while above the threshold bifurcation to another state with increasing (nonstationary) NO concentrations accompanied by a depletion of the OH and HO2 abundances takes place. 相似文献
17.
The results from a one-dimensional photochemical model of the troposphere representative of summertime conditions at Northern Hemisphere mid-latitudes are presented. A parameterization of mixing processes within the planetary boundary layer (PBL) has been incorporated into the model for both the daytime convective PBL and the formation of the nocturnal PBL. One result of the parameterized PBL is that the concentrations of some trace species in the free troposphere are 20–30% higher than when mixing processes are described by a vertical eddy diffusion coefficient which is held constant with respect to height and time.The calculations indicate that the lifetime of the oxides of nitrogen (NO
x
=NO+NO2) against photochemical conversion to nitric acid (HNO3) during summertime conditions is on the order of 6 h. This lifetime is short enough to deplete most of the NO
x
in the PBL, resulting in the finding that other reactive nitrogen species (HNO3 and peroxyacetyl nitrate) are more abundant than NO
x
throughout the free troposphere, even though NO
x
is the most abundant reactive nitrogen species at the surface. The effects of the inclusion of anthropogenic nonmethane hydrocarbon (NMHC) chemistry are also discussed. The inclusion of NMHC chemistry has a pronounced effect on the photochemistry of tropospheric oxone and increases thein situ column production by more than 30%. 相似文献