卫星遥感监测近地表细颗粒物多元回归方法研究

对地基监测PM2.5和气象数据、MODISAOD卫星数据与NCEP FNL数据进行了处理分析,在与一元简单线性模型(模型1)进行对比的基础上,建立了适应于北京及其附近地区遥感监测近地面颗粒物(PM2.5)浓度的多元线性(模型2)和非线性(模型3)回归模型,并对模型进行了评价验证和遥感监测初步应用.结果表明:模型1,2,3分别能够解释PM2.5 32.5%,56.1%,62.7%的变异.反演的PM2.5浓度与站点监测值相关性分别为0.5488(R2=0.3012),0.7449(R2=0.5549),0.7431(R2=0.5523).对于站点监测PM2.5浓度63.1652μg/m3的均值,反演均方根误差RMSE分别为43.5562,35.3321,36.8450μg/m3.模型2和3中气象因子分别能够解释PM2.5 23.6%和12.6%的变异,说明了气象因子影响北京地区春季PM2.5-AOD关系的显著性.3种模型整体上都不同程度地存在着低值高估和高值低估的现象.     

2008~2012年上海黑碳浓度变化特征分析

采用上海市城市环境气象中心2008~2012年黑碳质量浓度小时平均资料,分析了上海市区黑碳质量浓度变化规律.结果表明,2008~2012年间上海黑碳平均质量浓度呈下降趋势,各年黑碳平均质量浓度从(4 045.3±3 375.4)ng·m-3降至(2 766.2±2 078.9)ng·m-3,观测期间的逐年变化率分别为2.3%、-6.5%、-18.7%和-12.1%.与其它大城市相比,黑碳平均质量浓度为中等偏低水平.从年平均变化看,11和12月的5年平均质量浓度最高,分别为5 426.6 ng·m-3和5 365.3ng·m-3,其次为1、6和10月,分别为4 402.5、3 763.3和3 412.7 ng·m-3.工作日和休息日的5年平均日变化均呈明显双峰结构,两峰分别出现在北京时间07:00~10:00和18:00~22:00,工作日第一峰高于第二峰,休息日则相反.5年间,工作日黑碳平均质量浓度较休息日高9%.此外,根据有效观测数据,通过回归整理,给出了一个5年平均黑碳质量浓度日变化的逐时经验函数,以方便估计和预测黑碳浓度水平.     

西安冬季非灰霾天与灰霾天PM2.5中水溶性有机氮污染特征比较

2012年12月4~13日在西安市运用大流量大气采样器进行每小时1次PM2.5样品采集,对其进行有机碳(OC)、元素碳(EC)、水溶性有机碳(WSOC)、水溶性总氮(WSTN)、水溶性有机氮(WSON)以及无机离子分析,探讨其浓度、组成、时间变化特征和来源.结果表明,采样期间西安PM2.5中WSON小时平均浓度为(12±9.4)μg·m-3,最高达31μg·m-3,平均占水溶性总氮(WSTN)的47%±9.8%,而无机氮NH+4-N和NO-3-N则平均分别占WSTN的29%±8.5%和23%±8.1%.WSON∶WSOC(N∶C)质量比值范围为0.04~0.65,平均为0.31±0.13.在非灰霾天(能见度>10 km)、轻霾天(5 km<能见度<10 km)和重霾天(能见度<5 km),WSON分别为(1.6±0.9)、(6.5±3.9)和(23±4.7)μg·m-3.WSOC/OC质量比值在整个观测期间无明显变化,但是WSON/WSOC(N∶C)质量比值从非灰霾天、轻霾天到重霾天呈逐步增大趋势,其均值分别为0.2±0.1、0.3±0.1和0.4±0.1,与颗粒物碱度减弱酸度增强相一致.此外,整个采样期间WSON与NH+4、SO2-4和NO-3呈强线性相关(R2>0.80),阴阳离子当量平衡进一步显示:WSON与颗粒物中和度呈负相关(R2=0.53).研究结果表明,大气中有机胺等气态水溶性含氮有机物可通过酸碱中和与颗粒相酸性物质反应,由气相转移到颗粒相,并且重霾天低温、高湿和静风的气象条件有利于这种酸碱中和导致的气固相转化,促使更多的WSON生成.     

上海不同污染等级下气溶胶光学特性垂直分布特征

气溶胶光学特性是可吸入颗粒物的重要表征指标之一,而针对不同空气污染等级的气溶胶光学特性的垂直分布特征当前研究较少.本文利用上海地区(30°E,120°N~33°E,123°N)2006年6月至2011年12月的星载云-气溶胶激光雷达(Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations,CALIOPSO)资料分析不同季节气溶胶光学特性垂直分布的基础上,深入探讨了不同空气污染等级下的气溶胶垂直(0~6km)分布特征.结果表明:上海地区气溶胶粒子多聚集在0~2 km的高度上且具有明显的季节特征,冬春季节气溶胶粒子后向散射系数集中于0.005以上,颗粒物散射能力较大,其中冬季偏振比范围为0.15~0.25,色比范围为0.57~0.77,主要为不规则的小颗粒;夏季气溶胶粒子的偏振比(0.03~0.09)较小,气溶胶颗粒物较为规则;秋季各种形态的颗粒混合程度较高,其偏振比的范围为0.12~0.23,色比范围为0.58~0.90;不同污染等级下的气溶胶光学特性在垂直分布上具有明显的差异,在重污染时期散射能力大不规则颗粒物增多,垂直差异不明显,污染高度较高;轻度污染以规则颗粒物为主,颗粒物散射能力较小,表现出低层以粗颗粒为主,高层以细颗粒物为主的特征;轻微污染和无污染的气溶胶垂直分布类似,颗粒物散射能力较小.     

Online monitoring of water-soluble ionic composition of PM10 during early summer over Lanzhou City

Lanzhou is one of the most aerosol-polluted cities in China. In this study, an online analyzer for Monitoring for AeRosols and GAses was deployed to measure major water-soluble inorganic ions in PM10 at 1-hour time resolution, and 923 samples were obtained from Apr 1 to May 24, 2011. During the field campaign, air pollution days were encountered with Air Quality Index more than 100 and daily average concentration of PM10 exceeding 150 μg/m3. Based on the variation of water-soluble ions and results of Positive Matrix Factorization 3.0 model execution, the air pollution days were classified as crustal species- or secondary aerosol-induced, and the different formation mechanisms of these two air pollution types were studied. During the crustal species pollution days, the content of Ca2+increased and was about 2.3 times higher than the average on clear days, and the air parcel back trajectory was used to analyze the sources of crustal species. Data on sulfate, trace gases and meteorological factors were used to reveal the formation mechanism of secondary aerosol pollution. The sulfur oxidation ratio(SOR) was derived from the 923 samples, and the SOR had high positive correlation with relative humidity in early summer in Lanzhou.     

Identification of sources of lead in the atmosphere by chemical speciation using X-ray absorption near-edge structure (XANES) spectroscopy

Sources of Pb pollution in the local atmosphere together with Pb species, major ions, and heavy metal concentrations in a size-fractionated aerosol sample from Higashi-Hiroshima(Japan) have been determined by X-ray absorption near-edge structure(XANES) spectroscopy, ion chromatography, and ICP-MS/AES, respectively. About 80% of total Pb was concentrated in fine aerosol particles. Lead species in the coarse aerosol particles were PbC2O4, 2PbCO3·Pb(OH)2, and Pb(NO3)2, whereas Pb species in the fine aerosol particles were PbC2O4, PbSO4, and Pb(NO3)2. Chemical speciation and abundance data suggested that the source of Pb in the fine aerosol particles was different from that of the coarse ones. The dominant sources of Pb in the fine aerosol particles were judged to be fly ash from a municipal solid waste incinerator and heavy oil combustion. For the coarse aerosol particles, road dust was considered to be the main Pb source. In addition to Pb species, elemental concentrations in the aerosols were also determined. The results suggested that Pb species in size-fractionated aerosols can be used to identify the origin of aerosol particles in the atmosphere as an alternative to Pb isotope ratio measurement.     

Hygroscopicity of particles generated from photooxidation of α-pinene under different oxidation conditions in the presence of sulfate seed aerosols

Smog chamber experiments were conducted to investigate the hygroscopicity of particles generated from photooxidation of α-pinene/NOx with different sulfate seed aerosols or oxidation conditions. Hygroscopicity of particles was measured by a tandem differential mobility analyzer （TDMA） in terms of hygroscopic growth factor （Gf）, with a relative humidity of 85%. With sulfate seed aerosols present, Gf of the aerosols decreased very fast before notable secondary organic aerosols （SOA） formation was observed, indicating a heterogeneous process between inorganic seeds and organic products might take place as soon as oxidation begins, rather than only happening after gas-aerosol partition of organic products starts. The final SOA-coated sulfate particles had similar or lower Gf than seed-free SOA. The hygroscopicity of the final particles was not dependent on the thickness but on the hygroscopicity properties of the SOA, which were influenced by the initial sulfate seed particles. In the two designed aging processes, Gf of the particles increased more significantly with introduction of OH radical than with ozone. However, the hygroscopicity of SOA was very low even after a long time of aging, implying that either SOA aging in the chamber was very slow or the Gf of SOA did not change significantly in aging. Using an aerosol composition speciation monitor （ACSM） and matrix factorization （PMF） method, two factors for the components of SOA were identified, but the correlation between SOA hygroscopicity and the proportion of the more highly oxidized factor could be either positive or negative depending on the speciation of seed aerosols present.     

南宁市HJ-1CCD数据气溶胶光学厚度反演

利用环境一号卫星(HJ-1)CCD数据高时间分辨率、空间分辨率和宽覆盖的特点,进行城市地区气溶胶光学厚度定量反演研究。提出使用环境卫星数据自带的逐像元卫星观测角度文件及相应参数进行逐像元太阳天顶角、太阳方位角推算,生成四波段合成角度数据。结合改进后的暗目标算法,以及基于逐像元角度数据的6S查找表,对南宁市2014年1月14日、15日、16日HJ-1CCD数据进行气溶胶光学厚度反演。反演结果与ARONET地基观测数据进行验证,表明该算法有较高反演精度,相关系数为0.865,同时与MODIS气溶胶反演结果进行比较。结果表明,经过HJ-1CCD数据反演的气溶胶光学厚度可作为气溶胶时空分布的实时监测手段。     

影响北仑区域能见度的因素研究

利用对北仑区域内的气溶胶散射系数、气溶胶浓度、黑炭浓度以及NO2浓度的监测和分析,对区域影响能见度的的因素进行了研究,研究结果表明,影响能见度的消光系数主要由气溶胶的散射、气溶胶的吸收,干洁大气的散射和气态污染物的吸收四项组成,且组成比例总体稳定,但是,不同空气质量级别和灰霾天与非灰霾天之间的消光系数值及组成差异较大;通过对气溶胶与光散射系数的拟合得到,两者存在较好的正相关性。     

青岛大气气溶胶中铁的溶解度及其影响因素

大气气溶胶的干湿沉降带来的铁对海洋初级生产和固碳能力有着重要影响,但这种影响从根本上决定于沉降铁的溶解度.本文利用2012年12月在青岛连续采集的31个总悬浮颗粒物(TSP)样品,分析了其中微量元素Fe的总浓度和溶解态浓度,讨论了颗粒物浓度、气溶胶来源及酸化过程对Fe溶解度的影响.结果表明,气溶胶中Fe的总浓度和溶解态浓度分别为(3248±1683)ng·m-3和(43.3±16.4)ng·m-3,溶解度为0.57%~4.86%,平均为1.63%±1.02%.随着气溶胶中总Fe浓度的增加,Fe溶解度呈现规律性降低.气溶胶中Fe的溶解度与富集因子(EF)无相关关系,而与无机和有机酸性离子存在显著正相关关系.气团后向轨迹的聚类分析显示,观测期间,64.5%的气溶胶样品主要受北方沙尘源(DS)影响,35.5%的样品主要受到华北城市群等人为源(AS)影响.AS样品中Fe的溶解度平均为2.06%,高于DS样品中的1.36%.两组样品中Fe的EF值相当,但AS样品中酸性离子与溶解度的相关关系明显好于DS组,表明酸化过程可能是造成两组样品Fe溶解度差异的主要原因.