中国地区低对流层高层大气化学与长距离输送特征研究
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摘要
了解低对流层高层空气(海拔约1000～4000米高度)的污染特征及其物理化学变化过程对于认识人类活动对区域甚至全球尺度大气环境的影响具有重要意义。本研究通过在我国西北瓦里关山、华北泰山以及华南衡山开展高山观测,在东北吉林、西北甘肃、华东山东、江苏等地开展飞机航测,对主要的大气污染物进行了测量,并利用多种统计方法和分析手段如大气光化学箱模型、气流轨迹分析和聚类分析等对实验数据进行分析,研究了我国典型地区低对流层高层空气的污染状况、时空变化特征及其相关的大气化学过程与长距离输送特征。
基于观测实验所获得的第一手数据,本研究系统掌握了我国上述典型地区低对流层高层大气的污染水平与时空变化特征。作为我国的大气本底,瓦里关的大气污染物浓度普遍较低,但在某种条件下也可受到人为污染长距离输送的影响。主要污染物均呈现春季浓度高、夏季浓度低的季节变化特征和白天浓度低、夜间浓度高的日变化趋势。与之相比,泰山和衡山的大气污染物浓度则显著较高,明显受到了人为污染的影响。尤其是泰山,其主要一次污染物浓度高达瓦里关和部分欧美高山站点的几倍到几十倍,表明华北地区低对流层高层的空气污染已十分严重。受日间边界层发展以及山谷风的影响,泰山和衡山的主要污染物均呈现出下午浓度高、夜间浓度低的日变化特征。
研究还发现我国东北吉林地区夏季的高空云水已明显酸化,样品的平均pH值约为4.93。硫酸根和硝酸根为主要的致酸离子,二者的当量比约为2.1。对比同步采集的高空云水和地面降水样品发现,云下冲刷过程可对该地区的降水酸度起到一定的中和作用。此外,通过对比本研究与PEM-WestB和TRACE-P飞机航测实验关于几种关键卤代烃的观测资料发现,1994-2007年间中国-西北太平洋地区自由对流层大气中CH3CCl3、CCl4和C2Cl4的浓度均呈现持续下降的趋势,说明我国加入《蒙特利尔公约》后所采取的控制措施已取得较好效果。
通过后向气流轨迹聚类分析,本研究查明了瓦里关夏季大气来源的气候态长距离输送规律,并分析了其年际变化。发现瓦里关夏季来自东部的气流较多,气团在抵达前于低空经过了我国中、东部等人口密集、经济发达的地区；进一步研究发现这些气团具有较高的臭氧生成效率(7.7～11.3 ppbv/ppbv),因此我国东部地区人类活动排放的污染物向西长距离输送对瓦里关乃至整个青藏高原的大气臭氧(及其它微量成分)具有重要贡献。应用MCM光化学箱模式模拟了瓦里关的现场大气光化学反应过程,发现春、夏季的大气光化学反应均可导致03净生成,日间O3的平均生成速率分别约为0.30 ppbv/h和0.26 ppbv/h。HO2与NO反应是导致03化学生成的主要反应,而03的化学消耗则主要来自03的光解反应,其次为O3与自由基OH和HO2的反应。
通过对大气总氮氧化物(NOy)及其主要组成物种(包括NO、N02、HN03、aerosol NO3和PAN)进行测量,本研究查明了瓦里关、泰山和衡山大气中反应性氮氧化物的组成特征。上述我国典型地区的大气反应性氮氧化物均主要以硝酸(盐)的形式存在,表明在我国特定的大气环境中氮氧化物的化学转化以参与无机反应生成硝酸(盐)为主。研究也发现上述地区的氮氧化物组成特征各不相同,反映了我国不同地区具有各自独特的大气化学过程。研究同时认识了泰山和衡山典型季节大气气溶胶NO3-的粒径分布特征：泰山春、夏季气溶胶NO3-均呈粗、细双模态分布,且粗、细粒子中的浓度基本相当,而衡山春季气溶胶NO3-主要分布于粗模态中。
利用后向气流轨迹聚类分析,本研究还查明了泰山和衡山典型季节的大气长距离输送特征。春季泰山地区主要受到来自华北平原西部和北部地区污染物区域输送的影响；而夏季则主要受来自华北平原西南部以及鲁东胶东半岛地区污染物区域输送的影响。华东(包括华北平原和长三角)、珠三角以及衡山北部地区污染物的跨界传输是春季影响衡山地区大气污染的重要来源。此外,夏季华北地区污染物的跨界传输是导致在东北地区自由对流层内观测到严重污染个例的主要原因。
本研究获得了我国东北、西北、华东和华北地区典型季节对流层低层二氧化硫(802)和颗粒物光散射系数(Bsp)的垂直分布廓线,也获得了东北地区对流层低层内多种非甲烷烃和卤代烃的垂直分布廓线。大部分组分均呈现地面浓度最高,随高度升高浓度逐渐降低的垂直分布特征。这些廓线将有助于对化学传输模式以及对大气成分卫星遥感产品的验证等。通过对比飞机航测结果与OMI边界层SO2反演产品,本研究初步评估了OMI卫星在我国开展8O2空间遥感的表现,发现OMI二级产品可以较好地区分不同地区的8O2污染状况,但在污染极为严重的山东济南地区,OMI反演产品明显低估了实际的SO2浓度。
The pollution characteristics, atmospheric chemistry and transport at high altitudes in the lower troposphere (i.e.1000～4000 m a.s.l.) are crucial for understanding the influences of anthropogenic forcing on the regional and even global atmosphere. In the present study, several intensive field campaigns were carried out at Mt. Waliguan (100.90°E,36.28°E,3816 m a.s.l.) in western China, Mt. Tai (117.10°E, 36.25°E,1532 m a.s.l.) in northern China and Mt. Heng (112.70°E,27.30°E,1269 m a.s.l.) in southern China. Aircraft studies were also conducted over northeast (Jilin), northwest (Gansu) and central eastern China (Shandong and Jiangsu). During these experiments, large suites of air pollutants were measured. The data was analyzed with the aid of many statistical tools and modeling techniques including a photochemical box model, a backward trajectory model and cluster analysis. The results developed some better understandings of the pollution situation, chemical transformation and transport processes in the elevated lower troposphere over China.
Based on the firsthand observational data, this study provides a whole knowledge on the levels and temporal-spatial variations of air pollution at high altitudes in the lower troposphere over typical regions of China. As China's atmospheric baseline, the concentrations of air pollutants at Mt. Waliguan are generally low. However, it can also be affected to some extent by the long range transport of anthropogenic pollution. Major pollutants showed a well-defined seasonal pattern with higher concentrations in spring and lower levels in summer, and a unique diurnal profile with lower mixing ratios during the day and higher values at night. In comparison, the concentrations of air pollutants at Mt. Tai and Mt. Heng are substantially high, indicating more influences from anthropogenic activities. In particular, the abundances of primary pollutants at Mt. Tai are several to dozens of times higher than those at Mt. Waliguan and some European and American mountainous sites, demonstrating that air pollution at high altitudes over North China are quite serious. Affected by evolution of the boundary layer and mountain-valley breeze, all the major pollutants at Mt. Tai and Mt. Heng presented diurnal variations with the mixing ratios being the highest in the afternoon and the lowest at night.
We also found that the cloud water over northeast China (Jilin) had been evidently acidified with the mean pH value of～4.93. The dominant anion ions were SO42- and NO3- with the equivalent ratio of～2.1. Comparison of the cloud sample with the concurrent precipitation at the ground level suggested that the wash-out process can neutralize the acidity of rainfalls over this area. In addition, by comparing the results of several key halocarbons with the earlier PEM-West B (1994) and TRACE-P (2001) aircraft studies, continuous declining trends were derived for methyl chloroform (CH3CCl3), tetrachloromethane (CCl4) and tetrachloroethene (C2Cl4) over the great China-northwestern Pacific region. These results indicate the accomplishment of China in reducing these ozone-depleting compounds under the Montreal protocol.
The summertime climatological transport pattern of air masses arriving at Mt. Waliguan was derived by the cluster analysis of backward trajectories. Air parcels originating from central and eastern China dominated the air flow at Mt. Waliguan in summer. The pollution plumes from central and eastern China also showed high ozone production efficiencies (7.7～11.3 ppbv/ppbv). These results suggest strong impacts of anthropogenic forcing on the surface ozone and other atmospheric trace constituents on the Qinghai-Tibetan Plateau. The chemical budget of ozone was estimated using a photochemical box model constrained by the measured time-profiles of trace gases and meteorological variables. In-situ atmospheric photochemistry can lead to net ozone production in both spring and summer, with the mean daytime net production rates of 0.30 and 0.26 ppb/h respectively. Reaction of NO with HO2 dominates the ozone production, while ozone chemical destruction is mainly contributed by its photolysis followed by the reactions with OH and HO2.
The partitioning of reactive nitrogen was investigated for the first time in China based on the measurements of total and speciated nitrogen oxides (i.e. NOy, NO, NO2, PAN, HNO3, and particulate NO3-) at Mt. Waliguan, Mt. Tai and Mt. Heng. Distinct NOy budgets were obtained at the above three stations, suggesting different chemical transformation processes in different areas. However, inorganic nitrate (i.e. HNO3+ aerosol NO3-) was the most abundant reactive nitrogen species in all the three sites, indicating the chemical evolution of nitrogen oxides was dominated by the inorganic reactions. The size distributions of particulate NO3- were also gained at Mt. Tai and Mt. Heng during the measurement campaigns. The results showed bimodal distributions of NO3- in both spring and summer at Mt. Tai, while NO3- was mainly presented in coarse particles in spring at Mt. Heng.
Backward trajectories were also calculated and categorized to learn about the long-range transport patterns of air masses reaching Mt. Tai and Mt. Heng during the field experiments. In spring 2007, Mt. Tai was mainly affected by regional transport of air pollution from the western and northern parts of north China plains (NCP), while in summer mostly influenced by the regional transport from the southwestern NCP and the eastern Shandong peninsula. In spring 2009, air pollutants at Mt. Heng were mostly transported from eastern China (including NCP and Yangtze River Delta), Pearl River Delta and the northern areas.
Vertical distributions of SO2 and aerosol scattering coefficients (Bsp) were determined by aircraft measurements over northeast, northwest and central eastern China. Altitude profiles of many non-methane hydrocarbons and halocarbons were also obtained over northeast China. Most compounds exhibited a typical negative profile of decreasing mixing ratios with increasing altitude, although the gradients differed with different species. These data can be used to validate the chemical transport models and satellite retrievals. The SO2 column concentrations determined from the in-situ aircraft measurements were compared with the Ozone Monitoring Instrument (OMI) SO2 retrievals. The results show that the OMI data could distinguish the varying levels of SO2 pollution in the study regions, but appeared to have underestimated the SO2 column in the highly polluted region of eastern China (e.g. Ji'nan).
基于观测实验所获得的第一手数据,本研究系统掌握了我国上述典型地区低对流层高层大气的污染水平与时空变化特征。作为我国的大气本底,瓦里关的大气污染物浓度普遍较低,但在某种条件下也可受到人为污染长距离输送的影响。主要污染物均呈现春季浓度高、夏季浓度低的季节变化特征和白天浓度低、夜间浓度高的日变化趋势。与之相比,泰山和衡山的大气污染物浓度则显著较高,明显受到了人为污染的影响。尤其是泰山,其主要一次污染物浓度高达瓦里关和部分欧美高山站点的几倍到几十倍,表明华北地区低对流层高层的空气污染已十分严重。受日间边界层发展以及山谷风的影响,泰山和衡山的主要污染物均呈现出下午浓度高、夜间浓度低的日变化特征。
研究还发现我国东北吉林地区夏季的高空云水已明显酸化,样品的平均pH值约为4.93。硫酸根和硝酸根为主要的致酸离子,二者的当量比约为2.1。对比同步采集的高空云水和地面降水样品发现,云下冲刷过程可对该地区的降水酸度起到一定的中和作用。此外,通过对比本研究与PEM-WestB和TRACE-P飞机航测实验关于几种关键卤代烃的观测资料发现,1994-2007年间中国-西北太平洋地区自由对流层大气中CH3CCl3、CCl4和C2Cl4的浓度均呈现持续下降的趋势,说明我国加入《蒙特利尔公约》后所采取的控制措施已取得较好效果。
通过后向气流轨迹聚类分析,本研究查明了瓦里关夏季大气来源的气候态长距离输送规律,并分析了其年际变化。发现瓦里关夏季来自东部的气流较多,气团在抵达前于低空经过了我国中、东部等人口密集、经济发达的地区；进一步研究发现这些气团具有较高的臭氧生成效率(7.7～11.3 ppbv/ppbv),因此我国东部地区人类活动排放的污染物向西长距离输送对瓦里关乃至整个青藏高原的大气臭氧(及其它微量成分)具有重要贡献。应用MCM光化学箱模式模拟了瓦里关的现场大气光化学反应过程,发现春、夏季的大气光化学反应均可导致03净生成,日间O3的平均生成速率分别约为0.30 ppbv/h和0.26 ppbv/h。HO2与NO反应是导致03化学生成的主要反应,而03的化学消耗则主要来自03的光解反应,其次为O3与自由基OH和HO2的反应。
通过对大气总氮氧化物(NOy)及其主要组成物种(包括NO、N02、HN03、aerosol NO3和PAN)进行测量,本研究查明了瓦里关、泰山和衡山大气中反应性氮氧化物的组成特征。上述我国典型地区的大气反应性氮氧化物均主要以硝酸(盐)的形式存在,表明在我国特定的大气环境中氮氧化物的化学转化以参与无机反应生成硝酸(盐)为主。研究也发现上述地区的氮氧化物组成特征各不相同,反映了我国不同地区具有各自独特的大气化学过程。研究同时认识了泰山和衡山典型季节大气气溶胶NO3-的粒径分布特征：泰山春、夏季气溶胶NO3-均呈粗、细双模态分布,且粗、细粒子中的浓度基本相当,而衡山春季气溶胶NO3-主要分布于粗模态中。
利用后向气流轨迹聚类分析,本研究还查明了泰山和衡山典型季节的大气长距离输送特征。春季泰山地区主要受到来自华北平原西部和北部地区污染物区域输送的影响；而夏季则主要受来自华北平原西南部以及鲁东胶东半岛地区污染物区域输送的影响。华东(包括华北平原和长三角)、珠三角以及衡山北部地区污染物的跨界传输是春季影响衡山地区大气污染的重要来源。此外,夏季华北地区污染物的跨界传输是导致在东北地区自由对流层内观测到严重污染个例的主要原因。
本研究获得了我国东北、西北、华东和华北地区典型季节对流层低层二氧化硫(802)和颗粒物光散射系数(Bsp)的垂直分布廓线,也获得了东北地区对流层低层内多种非甲烷烃和卤代烃的垂直分布廓线。大部分组分均呈现地面浓度最高,随高度升高浓度逐渐降低的垂直分布特征。这些廓线将有助于对化学传输模式以及对大气成分卫星遥感产品的验证等。通过对比飞机航测结果与OMI边界层SO2反演产品,本研究初步评估了OMI卫星在我国开展8O2空间遥感的表现,发现OMI二级产品可以较好地区分不同地区的8O2污染状况,但在污染极为严重的山东济南地区,OMI反演产品明显低估了实际的SO2浓度。
The pollution characteristics, atmospheric chemistry and transport at high altitudes in the lower troposphere (i.e.1000～4000 m a.s.l.) are crucial for understanding the influences of anthropogenic forcing on the regional and even global atmosphere. In the present study, several intensive field campaigns were carried out at Mt. Waliguan (100.90°E,36.28°E,3816 m a.s.l.) in western China, Mt. Tai (117.10°E, 36.25°E,1532 m a.s.l.) in northern China and Mt. Heng (112.70°E,27.30°E,1269 m a.s.l.) in southern China. Aircraft studies were also conducted over northeast (Jilin), northwest (Gansu) and central eastern China (Shandong and Jiangsu). During these experiments, large suites of air pollutants were measured. The data was analyzed with the aid of many statistical tools and modeling techniques including a photochemical box model, a backward trajectory model and cluster analysis. The results developed some better understandings of the pollution situation, chemical transformation and transport processes in the elevated lower troposphere over China.
Based on the firsthand observational data, this study provides a whole knowledge on the levels and temporal-spatial variations of air pollution at high altitudes in the lower troposphere over typical regions of China. As China's atmospheric baseline, the concentrations of air pollutants at Mt. Waliguan are generally low. However, it can also be affected to some extent by the long range transport of anthropogenic pollution. Major pollutants showed a well-defined seasonal pattern with higher concentrations in spring and lower levels in summer, and a unique diurnal profile with lower mixing ratios during the day and higher values at night. In comparison, the concentrations of air pollutants at Mt. Tai and Mt. Heng are substantially high, indicating more influences from anthropogenic activities. In particular, the abundances of primary pollutants at Mt. Tai are several to dozens of times higher than those at Mt. Waliguan and some European and American mountainous sites, demonstrating that air pollution at high altitudes over North China are quite serious. Affected by evolution of the boundary layer and mountain-valley breeze, all the major pollutants at Mt. Tai and Mt. Heng presented diurnal variations with the mixing ratios being the highest in the afternoon and the lowest at night.
We also found that the cloud water over northeast China (Jilin) had been evidently acidified with the mean pH value of～4.93. The dominant anion ions were SO42- and NO3- with the equivalent ratio of～2.1. Comparison of the cloud sample with the concurrent precipitation at the ground level suggested that the wash-out process can neutralize the acidity of rainfalls over this area. In addition, by comparing the results of several key halocarbons with the earlier PEM-West B (1994) and TRACE-P (2001) aircraft studies, continuous declining trends were derived for methyl chloroform (CH3CCl3), tetrachloromethane (CCl4) and tetrachloroethene (C2Cl4) over the great China-northwestern Pacific region. These results indicate the accomplishment of China in reducing these ozone-depleting compounds under the Montreal protocol.
The summertime climatological transport pattern of air masses arriving at Mt. Waliguan was derived by the cluster analysis of backward trajectories. Air parcels originating from central and eastern China dominated the air flow at Mt. Waliguan in summer. The pollution plumes from central and eastern China also showed high ozone production efficiencies (7.7～11.3 ppbv/ppbv). These results suggest strong impacts of anthropogenic forcing on the surface ozone and other atmospheric trace constituents on the Qinghai-Tibetan Plateau. The chemical budget of ozone was estimated using a photochemical box model constrained by the measured time-profiles of trace gases and meteorological variables. In-situ atmospheric photochemistry can lead to net ozone production in both spring and summer, with the mean daytime net production rates of 0.30 and 0.26 ppb/h respectively. Reaction of NO with HO2 dominates the ozone production, while ozone chemical destruction is mainly contributed by its photolysis followed by the reactions with OH and HO2.
The partitioning of reactive nitrogen was investigated for the first time in China based on the measurements of total and speciated nitrogen oxides (i.e. NOy, NO, NO2, PAN, HNO3, and particulate NO3-) at Mt. Waliguan, Mt. Tai and Mt. Heng. Distinct NOy budgets were obtained at the above three stations, suggesting different chemical transformation processes in different areas. However, inorganic nitrate (i.e. HNO3+ aerosol NO3-) was the most abundant reactive nitrogen species in all the three sites, indicating the chemical evolution of nitrogen oxides was dominated by the inorganic reactions. The size distributions of particulate NO3- were also gained at Mt. Tai and Mt. Heng during the measurement campaigns. The results showed bimodal distributions of NO3- in both spring and summer at Mt. Tai, while NO3- was mainly presented in coarse particles in spring at Mt. Heng.
Backward trajectories were also calculated and categorized to learn about the long-range transport patterns of air masses reaching Mt. Tai and Mt. Heng during the field experiments. In spring 2007, Mt. Tai was mainly affected by regional transport of air pollution from the western and northern parts of north China plains (NCP), while in summer mostly influenced by the regional transport from the southwestern NCP and the eastern Shandong peninsula. In spring 2009, air pollutants at Mt. Heng were mostly transported from eastern China (including NCP and Yangtze River Delta), Pearl River Delta and the northern areas.
Vertical distributions of SO2 and aerosol scattering coefficients (Bsp) were determined by aircraft measurements over northeast, northwest and central eastern China. Altitude profiles of many non-methane hydrocarbons and halocarbons were also obtained over northeast China. Most compounds exhibited a typical negative profile of decreasing mixing ratios with increasing altitude, although the gradients differed with different species. These data can be used to validate the chemical transport models and satellite retrievals. The SO2 column concentrations determined from the in-situ aircraft measurements were compared with the Ozone Monitoring Instrument (OMI) SO2 retrievals. The results show that the OMI data could distinguish the varying levels of SO2 pollution in the study regions, but appeared to have underestimated the SO2 column in the highly polluted region of eastern China (e.g. Ji'nan).
引文
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