青岛大气臭氧及其前体物时间变化与污染特征

利用2003年12月—2005年3月青岛八关山观测资料,分析大气中O3、NOX和CO浓度时间变化规律与影响因素,探讨O3及其主要前体物NOX、CO间复杂的相互作用及相关关系。结果表明:青岛NO2日平均浓度年超标率为25%;受光化学反应及大气运动等影响,NOX与CO浓度为冬季高、夏季低,O3与之相反;NOX与CO浓度日变化呈双峰型分布,日间高于夜间;O3浓度峰值出现于午后(滞后于NOX约5 h),阴雨天夜间浓度出现回升。经滞后相关分析,NOX对O3浓度变化的累积效应作用时间为5—6 h;O3与NO、NO2浓度比值可较明显地验证出辐射强度与尾气排放对青岛及其他地区污染特征的影响。青岛CO与NOX比值在不同天气条件下维持在10.0左右,可用于定性估计其大气污染特征。     

影响北京夏季O3污染的O3前体物浓度及天气条件分析

根据2003年北京夏季近地面大气光化学污染物观测资料,对中国气象局培训中心(代表站)O3超标日浓度、O3前体物浓度、不同天气条件下O3浓度分布特征等进行分析。结果表明:中国北京夏季NO2,NO,CO的浓度特征与日本神奈川县相似,白天(16:00以前)如果NO2/NO超过29,则容易出现O3超标;VOC浓度的高低影响O3浓度;当处于暖湿气流控制,地面为小风或静风、气温较高、湿度较大的多云天气时,易出现O3超标情况。这些污染物发生的特点和规律对北京大气光化学污染的研究和防治具有借鉴意义。     

平流层大气过程研究的前沿与重要性

当前全球气候变化,重大灾害性天气气候事件的预警预测,以臭氧洞出现和臭氧层变化引起的全球环境变化监测预测,以及对临近空间的开发利用已经引起大气科学界对处于对流层大气以上的平流层大气过程的重要关注。扼要介绍了当前这方面的研究前沿和重要应用领域,最后提出我国加强平流层大气过程研究的建议。     

北半球10 hPa极地涡旋环流指数定义及分析

利用NCEP/NCAR再分析值10 hPa月平均高度场资料定义和计算了1948-2007年北半球10 hPa极地涡旋的强度指数(P)、 面积指数(S)和中心位置指数(λc, φc)。用它们分析了北半球10 hPa极地涡旋的季节变化和年际异常规律, 研究了它们与全球增暖、 臭氧（O3）异常和极地涛动（AO）的关系。结果表明： (1）北半球10 hPa层高纬6~8月为反气旋（A）控制; 9月~3月为气旋（C）控制。春季环流转型（C→A）缓慢; 秋季转型（A→C）迅速。(2）P、 S异常的年际变化具有同步性, 故异常分析仅取P进行。隆冬（1月）P的异常主要表现为年际尺度（10年以下周期）振荡, 不存在明显的年代际变化; 盛夏（7月）极地反气旋强度年代际变化显著。(3）隆冬极地气旋中心位置的异常明显大于盛夏反气旋。(4）极区中平流层平均气温的演变1、 7月迥异, 但它们与P的演变同步; 与全球增暖趋势无显著相关, 但7月P与O3异常有显著正相关。(5）隆冬（1月）10 hPa气旋强度指数P与极地涛动指数AO存在显著正相关, 故可用10 hPa ′表示AO。     

Evaluation of surface ozone measurements during 2000–2005 at a rural area in the upper Spanish plateau

This paper presents the main experimental results of surface ozone concentrations measured at a rural area in Northern Spain from February 2000 to December 2005. Daily and seasonal variation of ozone has been analysed. The peak concentration levels are obtained in the afternoon, mean value around 88 μg m⁻³, with extreme average values of 59 μg m⁻³ in January and 113 μg m⁻³ in July. Small differences are found in the mean and median of the ozone levels from April to August, when spring and summer maxima are observed. Despite the great inter-annual ozone variability obtained, most air quality indicators showed a positive trend. Further analysis of the monthly mean ozone concentrations of the main percentiles have also been performed using a harmonic model. The upward trend was 6.2 ± 1.7 μg m⁻³ for the 98th percentile. To interpret the main features of the annual cycle and describe the ozone peaks, the influence of meteorological factors is studied. In summer, ozone production is governed by local processes, air temperature being the major controlling factor. However, the origin of the spring maximum is not so well identified.     

The Northern Path of Asian Dust Transport from the Gobi Desert to North America

The aerosol index (AI) of the Total Ozone Mapping Spectrometer (TOMS) satellite data (1979 2001) was analyzed to reveal the climatological long-distance path of dust transport from Asia to North America. The AI in the west coast of the United States is highly correlated with that in the Gobi desert. Additionally, from the TOMS satellite images, it can be seen that very strong plumes advect from Asia to the west coast of North America in typical dust storm cases. When applying the sourcereceptor relationship to detect the northern dust transport path between the Gobi source region and the west coast of the United States receptor region, it is evident that the dust plume can be transported northward beyond 60°N from its source region and that it takes 5 to 6 days to reach the west coast of the United States. The cross correlation technique shown in this work is a useful tool that can be applied in other regions to give useful insights into relationships between major dust sources and downwind receptor locations by using remotely sensed dust observations.     

华北及其周边地区秋季气溶胶光学性质的星载和地基遥感观测

利用2004～2009年秋季臭氧监测仪的3级观测资料,分析了华北及周边地区的气溶胶光学性质。结果表明:大部分区域气溶胶光学厚度(Aerosol Optical Depth,AOD)和气溶胶紫外吸收指数(Ultra Violet Aerosol Index,UVAI)平均值分别高于0.8和0.75;高气溶胶事件发生频次统计表明,AOD高值(>0.4)频发于北京及其周边地区,UVAI高值(>1.0)频发于河北中部及南部地区;华北及其周边地区绝大多数城市平均AOD和UVAI分别高于0.7和0.60,而张家口、承德和阳泉3个城市的平均AOD和UVAI值分别低于0.6和0.65。作者进一步研究了2006年10月30日的一次霾事件中气溶胶的光学性质以及其时空分布特征。结果表明,霾由华北地区输送至渤海海域,并向东北方向输送;香河地基EZlidar激光雷达的垂直观测结果进一步表明,工业和城市型气溶胶主要集中在1500m以下,其中高浓度部分集中于650m以下,平均峰值位于285m,平均消光系数达2.15km-1;CALIOP卫星观测资料结合后向轨迹分析表明,大气低层气溶胶类型以工业和城市型气溶胶为主,而高层则由于上游大气输送沙尘粒子的混入使气溶胶类型转变为污染—沙尘型。霾事件期间,香河站CE-318太阳光度计观测的AOD平均值(标准差)从背景值0.08(0.04)升高至1.17(0.14);ngstrm指数平均值(标准差)从背景值0.90(0.10)升至1.12(0.09);核模态、积聚模态和粗模态的气溶胶粒子数柱总量均增加,其中细粒子所占比例明显升高。     

拉萨地区1998年夏季臭氧总量及垂直廓线的观测研究

该文根据1998年6~10月上旬在拉萨地区进行的臭氧总量及臭氧垂直廓线的观测结果, 并结合同期同纬度其他两个臭氧站数据资料, 证实了以拉萨地区为代表的青藏高原在夏季存在“臭氧低谷”的现象.分析表明, 地基和卫星观测的臭氧总量有一定误差. Umkehr观测反演结果表明夏季拉萨地区平流层臭氧分布和同纬度其他地区相比略有不同; 在对流层, 探空资料显示了该地区对流层臭氧有低值分布的特征.     

北京上空大气臭氧垂直分布的特征

利用我国自行研制的探空仪和地面接收设备首次较系统地获得了北京地区连续一年（2001年 3月至2002年 2月）的大气臭氧垂直分布资料。结果分析表明：①北京地区上空臭氧浓度极大值的季节均值的变化范围为15．1～16．7 mPa,其高度位于20．7～25．1km之间,极小值的季节均值的变化范围为 2．0～2．8 mPa,其高度在对流层顶附近。②边界层和平流层下部是臭氧浓度变化的活跃区域,并具有明显的季节变化,在边界层内夏季臭氧积分浓度高于冬季相应值的 1．7倍之多,而在平流层下部,冬季臭氧积分浓度则高于夏季的相应值。夏季边界层中臭氧浓度偏高,表明臭氧是北京地区夏季重要的污染气体之一。③北京上空臭氧垂直廓线的形态呈多样性,夏秋季节以单峰为主,冬春季节经常出现双峰和多峰结构;次峰出现的区域一般在10～18km高度范围内。     

Evaluation of alkene degradation in the detailed tropospheric chemistry mechanism, MCM v3, using environmental chamber data

The representation of alkene degradation in version 3 of the Master Chemical Mechanism (MCM v3) has been evaluated, using environmental chamber data on the photo-oxidation of ethene, propene, 1-butene and 1-hexene in the presence of NO_x, from up to five chambers at the Statewide Air Pollution Research Center (SAPRC) at the University of California. As part of this evaluation, it was necessary to include a representation of the reactions of the alkenes with O(³P), which are significant under chamber conditions but generally insignificant under atmospheric conditions. The simulations for the ethene and propene systems, in particular, were found to be sensitive to the branching ratios assigned to molecular and free radical forming pathways of the O(³P) reactions, with the extent of radical formation required for proper fitting of the model to the chamber data being substantially lower than the reported consensus. With this constraint, the MCM v3 mechanisms for ethene and propene generally performed well. The sensitivity of the simulations to the parameters applied to a series of other radical sources and sink reactions (radical formation from the alkene ozonolysis reactions and product carbonyl photolysis; radical removal from the reaction of OH with NO₂ and β-hydroxynitrate formation) were also considered, and the implications of these results are discussed. Evaluation of the MCM v3 1-butene and 1-hexene degradation mechanisms, using a more limited dataset from only one chamber, was found to be inconclusive. The results of sensitivity studies demonstrate that it is impossible to reconcile the simulated and observed formation of ozone in these systems for ranges of parameter values which can currently be justified on the basis of the literature. As a result of this work, gaps and uncertainties in the kinetic, mechanistic and chamber database are identified and discussed, in relation to both tropospheric chemistry and chemistry important under chamber conditions which may compromise the evaluation procedure, and recommendations are made for future experimental studies. Throughout the study, the performance of the MCM v3 chemistry was also simultaneously compared with that of the corresponding chemistry in the SAPRC-99 mechanism, which was developed and optimized in conjunction with the chamber datasets.