北京2013年1月连续强霾过程的污染特征及成因分析

以北京市2013年1月份连续灰霾天气中10~16日的强霾污染过程为例,利用MPL-4B型IDS系列微脉冲激光雷达观测资料由Fernald算法反演得到此次污染过程中气溶胶垂直分布特性,结合地面气象条件和天气形势分析污染原因,并讨论与气溶胶地面监测数据的符合性.结果表明:此次连续强霾过程污染严重,观测时段内89.4%的时间出现霾,39.8%的污染时段达到重度霾级别,其中大气地表消光系数与PM2.5浓度变化呈显著线性相关关系,相关系数达0.95.研究过程内,大气边界层在91%的时段低于500m,平均仅为293m,低边界层抑制了污染物的有效扩散;近地面垂向各高度的消光系数持续达到1.5km-1以上,对比气溶胶退偏比发现城市上空的大气强消光为气溶胶颗粒物和大气水分共同导致;气溶胶光学厚度(AOD,532nm)较大,有83.6%的时段超过1,且受相对湿度影响较大,相对湿度偏小时段的AOD值主要为气溶胶颗粒贡献,相对湿度较大时段,细颗粒物吸湿增长导致AOD受大气水分干扰显著.连续静稳的天气形势和区域污染是导致此次强霾发生和持续的主要原因,高湿天气则加剧了灰霾状况.     

基于无人机探空和数值模拟天津一次重污染过程分析

污染发生在边界层中,边界层热力和动力垂直结构对重污染天气形成有显著影响.本文基于无人机探空、地基遥感观测和数值模式,开展天津地区2019年1月10~15日重污染过程期间边界层垂直结构及污染成因分析,以期加强北方沿海城市边界层过程对重污染影响规律认知,提升重污染天气预报预警准确率.结果表明：大气温度层结对重污染天气形成、持续和消散有显著影响,此次过程伴随逆温层的发展和消散,PM_2.5高浓度区白天向大气上层发展,高度可达300 m以上,夜间向近地面压缩,高度在100 m左右;雾天气出现并在白天维持,改变了边界层垂直结构特征,雾顶逆温的持续存在抑制了污染物向大气上层扩散,使得白天湍流垂直混合过程贡献明显下降,导致近地面重污染天气维持和发展;过程期间区域输送贡献率为66.6%,边界层垂直结构与重污染天气区域输送密切相关,区域污染物输送高度主要出现在边界层顶部以及雾顶逆温层以上的大风速层处,且随着边界层和雾顶抬升高度的变化,通过下沉运动影响地面,形成北部弱高压天气控制下静稳天气区域输送;边界层垂直结构影响冷空气对空气质量的改善效果,S3阶段雾顶的强逆温导致冷空气无法通过湍流切应力传导到地面,在高低空存在明显的风速差,冷空气影响地面时间延后,作用减弱,重污染天气无法彻底缓解.     

利用微脉冲激光雷达分析上海地区一次灰霾过程

通过分析2008年6月至2009年5月期间浦东新区灰霾天气出现的特征,并以2008年12月19日至2008年12月21日一次典型的灰霾天气过程为例,利用激光雷达(Light laser detection and ranging,简称Lidar)数据资料反演得到气溶胶消光系数及其强度图和廓线图,结合地面气象数据和气溶胶观测资料,分析了此次灰霾天气形成的原因.一年的观测资料表明,上海地区冬季和春季易产生灰霾天气,冬季出现重度霾最多,秋季和夏季灰霾天气较少.较弱的太阳辐射以及静风、小风是导致灰霾天气发生的重要原因,且高湿度的霾天气对能见度影响更大.大气边界层(以下简称边界层)高度变化决定着灰霾天气发生的强度,当边界层高度在1km左右时,易发生轻微霾天气,当边界层高度降至600m左右时,易发生中度、重度霾天气,而太阳辐射强度变化决定着边界层高度的变化.轻微霾天气下,大气气溶胶垂直分布最强消光值约为0.15km-1,而重霾天气下可达0.30km-1以上.本次霾过程还受地面颗粒物排放的影响,主要是PM1和PM2.5,且在消光作用中散射性气溶胶的贡献大于吸收性气溶胶.轻微霾天气下PM2.5浓度为50μg·m-3,黑碳浓度为5000ng·m-3,浊度为200Mm-1,而重度霾时则分别达到200μg·m-3、24000ng·m-3和1400Mm-1.随着此次霾的出现,整层大气气溶胶光学厚度(AOD,550nm)不断增加,在重度霾时达到0.6左右,Angstrom指数在重度霾时显著降低,表明有大颗粒物导入,说明此次重度霾天气的发生还与气溶胶的输送有关.     

石家庄冬季典型污染过程气溶胶激光雷达观测

基于2016年冬季石家庄市微脉冲气溶胶激光雷达观测资料,采用归一化梯度法和梯度法两种方法反演了大气污染边界层高度,并将结果与相同时段探空资料获得的边界层高度进行对比验证,同时选取典型个例对污染边界层高度的过程演变特征进行了分析,探索了不同污染等级下污染边界层结构.结果表明,归一化、梯度法反演结果均与探空位温确定的边界层高度存在一致性,相关系数分别为0.62、0.55,均通过了0.05的显著性检验,但归一化相对误差为19%,梯度法为34%,表明归一化梯度法优于梯度法且其反演结果是可靠的.空气质量优良日,归一化梯度法反演结果准确度降低,与位温确定边界层高度最大偏差约1000m;随着污染程度加重,反演结果与位温确定边界层高度差减小,污染期间,污染边界层高度总体低于1000m,污染最重时段降到400m左右.不同空气质量等级、不同高度气溶胶消光系数垂直递减率具有明显差异,污染天气400m高度垂直递减率最大,表明该层以下为较重污染聚积层,之后随高度升高消光系数明显减小,700m以上为清洁空气.     

石家庄冬季典型污染过程气溶胶激光雷达观测

基于2016年冬季石家庄市微脉冲气溶胶激光雷达观测资料,采用归一化梯度法和梯度法两种方法反演了大气污染边界层高度,并将结果与相同时段探空资料获得的边界层高度进行对比验证,同时选取典型个例对污染边界层高度的过程演变特征进行了分析,探索了不同污染等级下污染边界层结构.结果表明,归一化、梯度法反演结果均与探空位温确定的边界层高度存在一致性,相关系数分别为0.62、0.55,均通过了0.05的显著性检验,但归一化相对误差为19%,梯度法为34%,表明归一化梯度法优于梯度法且其反演结果是可靠的.空气质量优良日,归一化梯度法反演结果准确度降低,与位温确定边界层高度最大偏差约1000m;随着污染程度加重,反演结果与位温确定边界层高度差减小,污染期间,污染边界层高度总体低于1000m,污染最重时段降到400m左右.不同空气质量等级、不同高度气溶胶消光系数垂直递减率具有明显差异,污染天气400m高度垂直递减率最大,表明该层以下为较重污染聚积层,之后随高度升高消光系数明显减小,700m以上为清洁空气.     

北京市区夏季O3生成过程分析

采用三维空气质量模型CMAQ-MADRID对北京地区夏季O3进行模拟,利用过程分析模块IPR和IRR研究北京市区大气O3的生成过程,重点分析自由基循环和NOx循环的量化特征.结果表明,市区整个边界层具有较强的大气氧化性,O3生成呈现VOC控制的特征.边界层内O3大气化学过程存在垂直差异,O3生成高值区在200～800m之间,近地层O3浓度升高主要依赖边界层内高层大气O3的垂直输送.NOx排放集中在近地层,新NO注入量较高,NOx循环次数仅为1.3,O3生成量很低.边界层上层大气从低层获得NOx,由于新NO注入量较低,同时上层大气保持了较强的大气氧化性,NOx循环次数达到5.0,O3生成量较高.     

车载激光雷达对北京地区边界层污染监测研究

介绍了自行研制的车载差分激光雷达AML-2探测原理及技术参数,于2006-08、2006-09在不同天气因素条件下对北京西南郊榆垡地区大气边界层污染物O3、NO2、SO2进行了实时监测,对比分析了3种污染物浓度垂直分布及日变化特征.结果表明,无外来污染输送时,3种污染物在阴雨天气总体浓度较小,O3和NO2浓度随高度升高而减小,SO2浓度垂直分布少见此特征,但在近地面0.6 km左右有较强SO2污染层.南部气流输送对北京地区大气环境影响明显,2006-08-23～2006-08-25这次强污染气流输送高度约1～1.5 km,3种污染物浓度垂直分布及日变化特征受到干扰,北京榆垡地区边界层O3、NO2、SO2总体浓度明显上升.     

基于车载雷达探测的一次华北冬季重污染天气成因研究

基于车载微脉冲气溶胶激光雷达、多普勒风廓线激光雷达和扭转拉曼廓线激光雷达的中山大学环境气象综合观测车,于2018年12月18日-22日在河北省望都县PM_2.5重污染期间开展定点观测.结合地面PM_2.5浓度和气象要素观测资料,对本次污染过程的成因展开分析.本次重污染过程日均PM_2.5浓度为163.2μg·m^-3,PM_2.5浓度的日变化特征明显,表现为白天PM_2.5浓度降低,傍晚至次日早晨PM_2.5浓度升高.气溶胶激光雷达观测结果发现,污染期间,700 m高度以下存在明显的消光系数高值区;夜间存在明显的消光系数高值区分层现象,气溶胶消光系数高值区出现高度可达1700 m.本次PM_2.5重污染过程受静稳边界层气象条件和高空气溶胶输送、沉降共同影响.在污染时段内,大气边界层低层小风持续,近地面和大气低层逆温和同温层频发,静稳边界层条件不利于PM_2.5的输送和扩散;此外,夜间高空气溶胶伴随强西风带出现...     

2018年3月两会期间北京重污染过程边界层气象的演变分析

为研究北京冬季重污染过程的污染特征及成因,采用边界层风场、温/湿场和气溶胶垂直探测等雷达综合遥测手段,对2018年3月北京两会期间的一次典型重污染过程,从边界层气象要素演变进行综合研究.结果表明:①整个污染过程历时7 d,轻度以上污染时数达118 h (占污染过程总小时数的69. 8%),严重污染时数达16 h (占污染过程总小时数的9. 5%),ρ(PM_(2.5))最高达333. 5μg/m~3.②从气溶胶的垂直空间演变来看,重污染天气的形成,除受本地源排放积累的影响外,还存在北京南部和东部的外部污染传输.贴地或上部逆温的稳定温度层结基本上对应ρ(PM_(2.5))的累积过程,其中,重污染时段逆温维持达68 h,逆温层厚度为500～1 100 m,最大平均逆温强度为0. 6℃/(100 m).大气边界层高度偏低(积累过程白天在1 000 m以下,夜间只有300～500 m),导致污染物持续积累.整个污染过程中,高湿时段引起PM2. 5吸湿增长和转化加重了污染程度;近地层持续小风导致污染积累;西南、东或东南方向大风层(10 m/s左右)向低空下探,有利于污染的缓解;强西北风或北风作用,使污染得以清除.研究显示,污染过程与边界层气象要素的演变密切相关.     

系留气球垂直观测平台的构建与应用

利用1 600 m~3车载系留气球,构建大气复合型污染垂直观测平台。利用该平台对近地大气边界层的多种气象要素、多种污染物浓度水平及其物理化学特性进行高分辨的垂直测量,用以研究大气边界层的形成和演变及大气污染物垂直分布和变化特征、大气光化学过程的垂直变化以及污染物的区域输送。该平台以0.5 m/s的速度进行升降,于2013年12月在上海成功应用于大气污染垂直观测,观测中共获取大气污染物有效廓线50余组。利用观测数据,初步探索上海近地层复合型大气污染的生消机制及大气污染物垂直分布特征,为上海市空气污染预警和防控对策机制的制定提供技术支撑。     

Effects of two sludge application on fractionation and phytotoxicity of zinc and copper in the soil

The potential harm of heavy metals is a primary concern in application of sludge to the agricultural land. A pot experiment was conducted to evaluate the effect of two sludges on fractionation of Zn and Cu in soil and their phytotoxicity to pakchoi. The loamy soil was mixed with 0%, 20%, 40%, 60% and 80% (by weight) of digested sewage sludge (SS) and composted sludge (SC). The additions of both sludges caused a significant raise in all fractions, resulting in that exchangeable (EXCH) and organic bound (OM) became predominance of Zn and organic bound Cu occupied the largest portion. There was more available amount of Zn and Cu in SS treatments than SC treatments. During the pot experiment, the concentration of Zn in EXCH, carbonate (CAR) and OM and Cu in EXCH and OM fractions decreased in all treatments, so their bioavailability reduced. Germination rate and plant biomass decreased when the addition rate was high and the best yield appeared in 20% mixtures at the harvest of pakchoi. The two sludges increased tissue contents of Zn and Cu especially in the SS treatments. Zn in pakchoi was not only in relationship to ΔEXCH and ΔCAR forms but also in ΔOM forms in the sludge-soil mixtures. Tissue content of Cu in pakchoi grown on SC-soils could not be predicted by ΔEXCH. These correlation rates between Zn and Cu accumulation in pakchoi and variation of different fractions increased with time, which might indicate that sludges represented stronger impacts on the plant in long-term land application.     

Intraspecific differences in effects of co-contamination of cadmium and

A hydroponic experiment was carried out to study intraspecific differences in the effects of different concentrations of cadmium (Cd)(0-10 mg/L) and arsenate (As(V)) (0-8 mg/L) on the growth parameters and accumulation of Cd and As in six wheat varieties Jing-9428, Duokang-1, Jingdong-11, Jing-411, Jingdong-8 and Zhongmai-8. The endpoints of wheat seedlings, including seed germination,biomass, root length and shoot height, decreased with increasing the Cd and As concentrations. Significant differences in seed germination, biomass, root length, shoot height and the accumulation of Cd and As were observed between the treatments and among the varieties (p ＜ 0.05). The lethal dosage 50% were about 20, 80, 60, 60, 80 and 20 mg As/L for Jing-9428, Duokang-1, Jingdong-11,Jing-411, Jingdong-8 and Zhongmai-8, respectively, and the corresponding values for Cd were about 30, 80, 20, 40, 60 and 10 mg Cd/L, respectively. Among the six varieties, Duokang-1 was found to be the most resistant to Cd and As toxicity, and Zhongmai-8 was the most sensitive to Cd and As co-contamination. The resistance of the six varieties was found dependant on the seedling uptake of Cd and As. Duokang-1 was the most suitable for cultivation in Cd and As co-contaminated soils.     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Degradation of metabolites accumulated of benzo[a]pyrene by coupling Penicillium Chrysogenum with KMnO4

Several main metabolites of benzo[a]pyrene （BaP） formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone （BP 1,6- quinone）, trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene （BP 7,8-diol）, 3-hydroxybenzo[a]pyrene （3-OHBP）, were identified by high-performance liquid chromatography （HPLC）. The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that （1） the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; （2） the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; （3） the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% （w/v）, concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.