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1.
Satellite measurements of tropospheric column O3 and NO2 in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O3 is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO2 is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O3 and NO2 fields. The analysis of the model results show that the industrial emission of NOx (NO + NO2) contributes about 50%–80% to tropospheric column NO2 in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NOx to tropospheric column O3 ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NOx emissions have a small effect on tropospheric O3 in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NOx on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.  相似文献   

2.
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   

3.
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   

4.
In this study, the chemical and physical losses of nitrogen oxides (NOx) over the Korean peninsula were discussed in order to better understand the effects of the NOx losses on the tropospheric NO2 columns. Initially, it was found that the physical loss processes due to dry and wet depositions had almost negligible impacts on the NOx loss processes over the Korean peninsula. In contrast, the hourly NOx chemical column losses were large at ??1014 molecules cm?2 h?1. The amounts of NOx removed for 1 hour account for approximately 33?C35% of the episode-averaged tropospheric NO2 columns during summer over the Korean peninsula. The NOx chemical column loss rates were 24.1?C70.9 times larger than the NOx physical column loss rates. In a budget analysis of the NOx chemical column losses, HNO3 formation via the reaction of OH + NO2 had the largest contribution toward the NOx chemical losses (42?C55% during fall and winter seasons; 76?C77% during spring; 92?C93% during summer). Large amounts of NOx were also removed by heterogeneous nitrate formation via N2O5 condensation during the cold seasons (42?C56%) over the Korean peninsula. The columnar NOx chemical losses took place mainly due to the two chemico-physical reaction processes, and also showed seasonal variations. PAN (Peroxyacetyl Nitrate) is another NO2 reservoir of potential importance. If the influence of the PAN-related chemistry on the NOx budget is considered, it can result in an approximate 69% increase in the NOx chemical column loss during summer. Such increases in the amounts of NOx removed for 1 hour due to the formation of PAN were equivalent to 56?C58% of the episode-averaged tropospheric NO2 columns during summer over the Korean peninsula. Such active NOx chemical losses during summer are another main factor for the tropospheric NO2 columns exhibiting their smallest values during summer.  相似文献   

5.
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   

6.
Using the global chemistry and transport model MOZART,the simulated distributions of tropospheric hydroxyl free radicals(OH) over China and its sensitivities to global emissions of carbon monoxide(CO),nitrogen oxide(NO x),and methane(CH 4) were investigated in this study.Due to various distributions of OH sources and sinks,the concentrations of tropospheric OH in east China are much greater than in west China.The contribution of NO + perhydroxyl radical(HO 2) reaction to OH production in east China is more pronounced than that in west China,and because of the higher reaction activity of non-methane volatile organic compounds(NMVOCs),the contributions to OH loss by NMVOCs exceed those of CO and take the dominant position in summer.The results of the sensitivity runs show a significant increase of tropospheric OH in east China from 1990 to 2000,and the trend continues.The positive effect of double emissions of NO x on OH is partly offset by the contrary effect of increased CO and CH 4 emissions:the double emissions of NO x will cause an increase of OH of 18.1%-30.1%,while the increases of CO and CH 4 will cause a decrease of OH of 12.2%-20.8% and 0.3%-3.0%,respectively.In turn,the lifetimes of CH 4,CO,and NO x will increase by 0.3%-3.1% with regard to double emissions of CH 4,13.9%-26.3% to double emissions of CO and decrease by 15.3%-23.2% to double emissions of NO x.  相似文献   

7.
大气污染物排放清单是空气质量模拟和空气污染治理的重要依据.本研究比较分析了两套覆盖江苏省的2017年大气污染物排放清单，即分别由上海市环境科学研究院、江苏省环境科学研究院编制的"长三角清单"和"江苏省清单"，并结合区域空气质量模型CMAQ评估不同清单对长三角地区2017年1、4、7、10月的空气质量模拟的影响.清单比较结果表明，除二氧化硫（SO2）以外，江苏省清单估算的各污染物排放量较长三角清单低.通过与观测数据比较，发现两套清单对SO2、氮氧化物（NOx）、臭氧（O3）和细颗粒物（PM2.5）的模型模拟性能均较好.江苏省清单与长三角清单两者的模拟结果空间分布接近，其中江苏省清单模拟的PM2.5和O3在长三角多数地区略低于长三角清单的模拟结果（1月O3除外）.江苏省清单与长三角清单均能够用于空气质量模式模拟，可为江苏地区的细颗粒物和光化学烟雾污染的控制策略制定提供参考.  相似文献   

8.
Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NOx mixing ratiosup to 300 pptv in February and for NOx mixing ratios up to 500 pptv in May. These NOx limits are an order of magnitude higher thanmedian NOx levels observed, illustrating the strong dependence ofgross ozone production rates on NOx mixing ratios for the majority of theobservations. The threshold NOx mixing ratio needed for netpositive ozone production was also calculated to increase from NOx 10pptv in February to 25 pptv in May, suggesting that the NOx levels needed to sustain net ozone production are lower in winter than spring. This lower NOx threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NOx neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.  相似文献   

9.
利用2010—2012年对流层臭氧（O3）及其多种前体物的卫星遥感资料和全球水汽再分析资料,研究东亚区域O3及其前体物的时空分布,以及在中国东部（分为南、北两部分）相关性的季节变化。结果表明:东亚区域NO2与CO的对流层柱含量均表现为冬季高、夏季低的时空变化形式。O3对流层柱含量夏季达到峰值,冬季为谷值。中国东部的北部与南部地区O3与NO2均在夏秋季呈正相关,冬春季呈负相关。夏季大部分地区NOx的光化学循环反应对O3生成有积极的促进作用,冬季大部分地区O3的光化学循环生成受到抑制。O3与CO在北部地区夏秋季和南部地区夏季正相关性最大,无论是在北部还是南部地区,O3与CO的相关性在轻污染情况下最大,而在重污染和背景情况下较小,表明重污染气团向下风方的输送更有利于O3的光化学生成。O3与水汽在北部和南部地区的多数时间均呈较显著的正相关性,而在南部地区夏季和北部地区冬季具有较大的负相关性,反映出不同的环流形式、气团来源及伴随的天气条件变化对O3分布的影响。  相似文献   

10.
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   

11.
Both surface environmental monitoring and satellite remote sensing show that North China is one of the regions that are heavily polluted by NO2. Using the NO2 monitoring data from 18 major cities in the region, the tropospheric NO2 column density data from the Ozone Monitoring Instrument (OMI) on the Aura satellite, and the observations from the China Meteorological Administration network, this paper analyzes a regional NO2 pollution event in February 2007 over North China, examines the convergence of the pollutant, and identies its correlation with the atmospheric background conditions. The results show that daily mean NO2 concentrations derived from surface observations are consistent with the mean values of the OMI measurements, with their correlation coeficient reaching 0.81. The correlations of NO2 concentration with general weather patterns and sequential changes of temperature structure from 925 hPa down to the surface indicate that the weather fronts, high pressure and low pressure systems in the atmosphere play a role in changing the temporal and spatial evolutions of NO2 through removing, accumulating or converging of the pollutant, respectively. It is also found that the eastern Taihang Mountains is most heavily polluted by NO2 in North China. Based on a model that correlates NO2 column density with surface wind vector, the relation of the NO2 concentrations in six major cities in North China to the surrounding wind field is analyzed. The results show that the maximum wind field is associated with the highest frequency of pollution events, and under certain large-scale atmospheric conditions together with the topographic effect, small- and meso-scale wind fields often act to transport and converge pollutants, and become a major factor in forming the heaviest NO2 pollution event in North China. Analysis of the causes for the severe NO2 pollution event in this study may shed light on understanding, forecasting, and mitigating occurrences of heavy NO2 pollution.  相似文献   

12.
Emissions may affect climate indirectly through chemical interactions in the atmosphere, but quantifications of such effects are difficult and uncertain due to incomplete knowledge and inadequate methods. A preliminary assessment of the climatic impact of changes in tropospheric O3 and CH4 in response to various emissions is given. For a 10% increase in the CH4 emissions the relative increase in concentration has been estimated to be 37% larger. The radiative forcing from enhanced levels of tropospheric O3 is estimated to 37% of the forcing from changes in CH4. Inclusion of indirect effects approximately doubles the climatic impact of CH4 emissions. Emissions of NOx increase tropospheric O3, while the levels of CH4 are reduced. For emissions of NOx from aircraft, the positive effects via O3 changes are significantly larger than the negative through changes in CH4. For NOx emitted from surface sources, the effects through changes in O3 and CH4 are estimated to be of similar magnitude and large uncertainty is connected to the sign of the net effect. Emissions of CO have positive indirect effects on climate through enhanced levels of tropospheric o3 and increased lifetime of CH4. These results form the basis for estimates of global warming potentials for sustained step increases in emissions.  相似文献   

13.
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   

14.
The new European Council Directive (PE-CONS 3696/07) frames the inhalable (PM10) and fine particles (PM2.5) on priority to chemically characterize these fractions in order to understand their possible relation with health effects. Considering this, PM2.5 was collected during four different seasons to evaluate the relative abundance of bulk elements (Cl, S, Si, Al, Br, Cu, Fe, Ti, Ca, K, Pb, Zn, Ni, Mn, Cr and V) and water soluble ions (F−, Cl−, NO2 −, NO3 −, SO4 2−, Na+, NH4 +, Ca2+ and Mg2+) over Menen, a Belgian city near the French border. The air quality over Menen is influenced by industrialized regions on both sides of the border. The most abundant ionic species were NO3 −, SO4 2− and NH4 +, and they showed distinct seasonal variation. The elevated levels of NO3 − during spring and summer were found to be related to the larger availability of the NOx precursor. The various elemental species analyzed were distinguished into crustal and anthropogenic source categories. The dominating elements were S and Cl in the PM2.5 particles. The anthropogenic fraction (e.g. Zn, Pb, and Cu) shows a more scattered abundance. Furthermore, the ions and elemental data were also processed using principal component analysis and cluster analysis to identify their sources and chemistry. These approach identifies anthropogenic (traffic and industrial) emissions as a major source for fine particles. The variations in the natural/anthropogenic fractions of PM2.5 were also found to be a function of meteorological conditions as well as of long-range transport of air masses from the industrialized regions of the continent. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

15.
利用中国科学院大气物理研究所香河大气探测综合试验站2010年3月至2012年2月(2年)的多轴差分吸收光谱仪(MAX-DOAS)观测数据和32 m高塔常规气象资料,反演了华北地区香河站对流层NO2柱浓度,分析了该区域NO2柱浓度的季节变化特征。研究表明:可见光455~485 nm、紫外330~370 nm都可以作为MAX-DOAS工作波段很好地反演NO2;香河地区NO2柱浓度夏季最低,几乎保持在2×1016 cm–2以下,春、秋季次之,在3×1016 cm–2上下小范围浮动,冬季最高,可达4.5×1016 cm–2;月平均最低值出现在7月,最高值出现在11月。NO2柱浓度与风速、风向密切相关:来自东边唐山方向的风,风速越大时NO2浓度越高,因为唐山是NO2的高值区之一;其它方向风速越大,浓度越低。春、夏两季NO2柱浓度日变化趋势比较平缓,秋、冬两季日变化明显,秋季正午偏高,冬季早晚偏高。  相似文献   

16.
Photochemical indicators for determination of O3–NOx–ROG sensitivity and their sensitivity to model parameters are studied for a variety of polluted conditions using a comprehensive mixed-phase chemistry box model and the novel automatic differentiation ADIFOR tool. The main chemical reaction pathways in all phases, interfacial mass transfer processes, and ambient physical parameters that affect the indicators are identified and analyzed. Condensed mixed-phase chemical mechanisms are derived from the sensitivity analysis.Our results show that cloud chemistry has a significant impact on the indicators and their sensitivities, particularly on those involving H2O2, HNO3, HCHO, and NOz. Caution should be taken when applying the established threshold values of indicators in regions with large cloud coverage. Among the commonly used indicators, NOy and O3/NOy are relatively insensitive to most model parameters, whereas indicators involving H2O2, HNO3, HCHO, and NOz are highly sensitive to changes in initial species concentrations, reaction rate constants, equilibrium constants, temperature, relative humidity, cloud droplet size, and cloud water content.  相似文献   

17.
The global three-dimensional Lagrangian chemistry-transport model STOCHEM has been used to follow the changes in the tropospheric distributions of the two major radiatively-active trace gases, methane and tropospheric ozone, following the emission of pulses of the short-lived tropospheric ozone precursor species, methane, carbon monoxide, NOx and hydrogen. The radiative impacts of NOx emissionswere dependent on the location chosen for the emission pulse, whether at the surface or in the upper troposphere or whether in the northern or southern hemispheres. Global warming potentials were derived for each of the short-lived tropospheric ozone precursor species by integrating the methane and tropospheric ozone responses over a 100 year time horizon. Indirect radiative forcing due to methane and tropospheric ozone changes appear to be significant for all of the tropospheric ozone precursor species studied. Whereas the radiative forcing from methane changes is likely to be dominated by methane emissions, that from tropospheric ozone changes is controlled by all the tropospheric ozone precursor gases, particularly NOxemissions. The indirect radiative forcing impacts of tropospheric ozone changes may be large enough such that ozone precursors should be considered in the basket of trace gases through which policy-makers aim to combat global climate change.  相似文献   

18.
Long-term measurements of ambient particulate matter less than 2.5 μm in diameter (PM2.5) and its chemical compositions were performed at a rural site in Korea from December 2005 to August 2009. The average PM2.5 concentration was 31 μg m−3 for the whole sampling period, and showed a slightly downward annual trend. The major components of PM2.5 were organic carbon, SO42−, NO3−, and NH4+, which accounted for 55 % of total PM2.5 mass on average. For the top 10 % of PM2.5 samples, anionic constituents and trace elements clearly increased while carbonaceous constituents and NH4+ remained relatively constant. Both Asian dust and fog events clearly increased PM2.5 concentrations, but affected its chemical composition differently. While trace elements significantly increased during Asian dust events, NO3−, NH4+ and Cl were dramatically enhanced during fog events due to the formation of saturated or supersaturated salt solution. The back-trajectory based model, PSCF (Potential Source Contribution Function) identified the major industrial areas in Eastern China as the possible source areas for the high PM2.5 concentrations at the sampling site. Using factor analysis, soil, combustion processes, non-metal manufacture, and secondary PM2.5 sources accounted for 77 % of the total explained variance.  相似文献   

19.
Previous zero-dimensional photochemical calculations indicate that multiple tropospheric steady states may exist, in which different NO x (NO+NO2) levels could be supported by the same source of NO x . To investigate this possibility more closely, a one-dimensional photochemical model has been used to estimate the rate of removal of atmospheric NO x compounds at different NO x levels. At low NO x levels NO x is photochemically converted to HNO3, which is removed by either wet or dry deposition. At high NO x levels formation of HNO3 is inhibited, and NO x is removed by a variety of other processes, including rainout of N2O4 and N2O5, surface deposition of NO and NO2, and direct dissolution of NO and NO2 in rainwater. Multiple steady states are possible if surface deposition of NO x is relatively inefficient. The NO x source required to trigger high atmospheric NO x levels is approximately 10 to 15 times the present global emission rate-less than half the source strength predicted by the zero-dimensional model. NO x mixing ratios in excess of 10-7 would cause severe damage to the ozone layer and could result in either a climatic warming or cooling, depending upon the amount of NO2 present.  相似文献   

20.
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   

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