环珠江口近地面夜间臭氧上升现象：基于垂直观测的两个个例研究

利用广州塔的O₃观测资料、风廓线雷达和转动拉曼温廓线激光雷达探测的垂直环境气象等观测资料,结合ERA5的近地面风场,对2017年5月6—7日(Case I)和2019年10月1—2日(CaseⅡ)两个典型个例从垂直混合与水平输送的角度进行特征与成因分析.O₃的垂直观测结果表明,夜间残留层可储存日间混合层内的高浓度O₃气团.从垂直混合与水平输送的分析结果表明,残留层O₃的垂直混合及高浓度O₃气团的水平输送是夜间地表O₃的重要来源：夜间存在垂直风切变或边界层抬升,均可加强O₃的垂直混合;珠三角地区背景风表现为在早上偏北风和晚上转换为偏南风,广州与佛山地表O₃浓度上升最显著.此外,夜间O₃浓度上升事件可造成夜间及凌晨O₃ 8 h滑动平均值持续高值,对空气质量和大气氧化性造成一定影响.     

夜间近地表臭氧观测

2018年12月15~18日使用激光雷达在河北望都观测气溶胶与O₃,利用气溶胶消光系数廓线判断边界层的变化,进而研究大气边界层对于近地表层（300m）O₃浓度的影响.结果表明,边界层主要影响O₃的干沉降以及高空O₃的垂直输送,在受本地污染控制时,近地表O₃浓度受干沉降控制明显,随着边界层高度的下降而减少;西北地区气团占主导时,O₃浓度主要受水平传输以及高空垂直输送影响.     

天津大气扩散条件对污染物垂直分布的影响研究

利用2017~2019年夏、冬季天津市大气污染物监测和气象观测数据,基于天津气象铁塔垂直观测,针对大气垂直扩散条件对PM_2.5和O₃的影响进行研究.结果显示:近地面PM_2.5浓度随高度的升高而下降,O₃浓度则随高度的升高而上升,受大气垂直扩散条件的季节和日变化影响,冬季,地面与120m PM_2.5质量浓度相关明显,与200m PM_2.5质量浓度无明显相关.夏季,120m和200m PM_2.5质量浓度相关系数为0.72,午后通常出现120m和200m PM_2.5质量浓度高于地面的情况.夏季,不同高度O₃浓度差异小于冬季,地面与120m高度O₃浓度接近.以大气稳定度、逆温强度和气温递减率作为大气垂直扩散指标,对地面PM_2.5和O₃垂直分布具有指示作用.冬季,TKE与PM_2.5质量浓度相关系数为到-0.65,夏季,TKE与ΔPM_2.5相关系数为-0.39.夏、冬季TKE与地面O₃浓度的相关系数分别为0.46和0.53,与ΔO₃的相关系数分别为0.73和0.70.弱下沉运动对地面O₃浓度影响较强,40m高度垂直运动速度与地面O₃浓度的相关系数在冬、夏季分别为-0.54和-0.61.对冬季典型PM_2.5重污染过程的分析发现,雾霾的生消维持和PM_2.5浓度的变化与大气稳定度、气温垂直递减率和TKE的变化有直接关系.对夏季典型O3污染过程的分析发现,近地面的O₃污染的形成与有利光化学反应的气象条件密切相关,同时,垂直向下输送和有利垂直扩散条件对O₃污染的形成和爆发影响明显.     

武清地区冬季一次重污染过程垂直分布特征

为研究京津冀地区重污染过程大气污染物的垂直分布特征,于2016年12月13日重污染前（11:49-12:18）和12月18日重污染期间（11:00-11:16）在北京市、天津市、河北省交界处的武清地区利用系留气球开展1 000 m以下的大气观测,探究污染物的垂直分布特征及对流边界层、覆盖逆温层和混合层等要素对重污染形成的影响.结果表明:①在重污染前,大气层结不稳定,ρ（PM_2.5）、ρ（NO_x）与ρ（O₃）随高度变化不明显,存在明显的垂直对流运动,有利于大气污染物的扩散;PM_2.5/PM₁₀[ρ（PM_2.5）/ρ（PM₁₀）]在800 m以下为0.60~0.80,在800~1 000 m以上大于0.90.②重污染期间,近地面大气层分为对流边界层（距地面0~150 m）、覆盖逆温层（150~370 m）、混合层（370~500 m）和自由大气（500 m以上）4个层次.③NO_x主要在对流边界层内聚积;高空O₃在向近地面扩散时受强混合层阻挡,在混合层出现一个小峰值;PM_2.5不仅在近地面聚积,而且在覆盖逆温层内聚积,ρ（PM_2.5）在覆盖逆温层内呈双峰（峰值分别出现在150和370 m）分布,其粒径集中在0.5~1.0 μm,属于积聚态气溶胶.研究显示,在不利扩散条件下,汽车排放、村镇居民供暖排放的污染物聚积及二次颗粒物的生成是重污染形成的重要因素.      

边界层方案与垂直混合对京津冀地区O3模拟的影响研究

采用WRF-Chem模式中的3种边界层方案YSU、MYJ和ACM2对2019年6月京津冀及周边地区典型O₃污染月份开展模拟研究.详细对比了各方案对地面气象要素、NO₂和O₃浓度时空分布,以及温湿风要素和O₃浓度垂直分布的模拟效果.结果表明：3种方案对地面气象要素的时空分布和温湿风要素的垂直变化模拟较为合理.MYJ方案模拟地面气象要素整体效果最佳.各方案对边界层高度的日变化特征模拟较好,相关系数为0.58~0.69,但存在白天偏高、夜间偏低的现象,YSU方案相比效果最佳.3种边界层方案对NO₂浓度模拟普遍高估,而O₃模拟结果则出现低估.白天模拟偏差较小而夜间偏差较显著.模拟最佳的是ACM2,其次为YSU和MYJ.3种方案均较好地模拟出了O₃的垂直分布特征,但整体低估了O₃浓度.对上午O₃垂直分布的模拟差异较下午更为明显.此外,基于YSU方案设置了3个敏感实验,通过调整化学模块所用的湍流扩散系数阈值,对比分析了垂直混合过程改变对O₃浓度模拟的影响,模拟的变化只反映由于边界层的垂直混合过程改变造成的污染差异,而不是由于热动力场的调整造成的变化.模拟结果表明3个方案均可改善区域上地面NO₂和O₃的模拟性能,尤其是对原3种边界层方案模拟O₃均明显低估的华北平原地区提升效果最显著,平均偏差降低了23.7%.在垂直方向上,湍流扩散系数阈值的调整增加了早间近地面模拟的O₃浓度,改善了模拟偏低的现象,但同时增大了高层O₃浓度的负偏差.敏感性方案显著改善了夜间的模拟,白天则并不明显.这些结果显示出湍流扩散系数对O₃垂直混合的重要影响.因此,改进湍流扩散系数的参数化对O₃模拟是必要的.     

深圳市秋季大气臭氧立体分布特征

利用大气O₃探测激光雷达在深圳市东部生态区和西部城区同步开展垂直观测,探究了2018年深圳市O₃立体分布在秋季光化学污染活跃期至冬季非活跃期的演变过程.结果表明：光化学反应活跃的10月,东部地面O₃浓度相对于西部地面高出约128%;地面向上至450m,O₃浓度在东部生态区发生快速降低,而在西部城区由于存在“滴定效应”,O₃浓度随高度升高而升高;450m~2km,东、西部O₃浓度均随高度升高而降低,西部城区O₃浓度水平超过东部生态区约30%;2km以上高空,东、西部O₃浓度趋同（70μg/m³）,并保持稳定,为具深圳市秋季O₃污染过程提供了较高的大气背景浓度.高污染期间,深圳市大气边界层内O₃浓度变化较为一致,西部高空的O₃区域传输作用更加显著.秋季至冬季光化学反应逐渐减弱,深圳市O₃浓度的水平和垂直空间差异逐渐减小,冬季的深圳市O₃污染基本受大气背景控制.     

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...     

深圳西部城区大气O3污染特征及超标成因

利用近5a深圳西部城区（大学城）大气臭氧（O₃）在线监测数据,结合深圳大学城超级站大气复合污染综合观测,获取了大气O₃演变趋势,并探究O₃超标日气象条件及其前体物的组成变化以期掌握大气O₃超标成因.结果表明,深圳大学城大气O₃日最大8h平均体积分数上升速度达1.1×10^-9/a,超标率达到6%以上.高温低湿的气象条件更容易促进大气O₃生成,高温时光化学反应强烈有利于O₃的本地生成,而低湿可能不利于O₃的湿去除从而导致污染积累.挥发性有机物（VOCs）不同组分在O₃超标日上升幅度（70%~95%）明显高于NOx（28%）,且O₃高值浓度分布在高VOCs低NOx区域,说明深圳大学城大气O₃生成主要受VOCs控制.O₃超标日的甲苯与苯比值（T/B）在夜间超过10表明可能存在大量工业排放;而含氧挥发性有机物（OVOCs）在午间（12：00~14：00）的消耗相较于非超标日高出了1倍左右,表明工业活动排放的OVOCs对白天O₃生成可能贡献显著.     

北京夏季典型臭氧污染分布特征及影响因子

为研究北京地区O₃分布特征及其影响因子,利用AML-3车载式大气环境污染激光雷达系统(下称AML-3)对北京地区2011年5月7日—6月9日的φ(O₃)进行观测. 通过AML-3自带的污染物地面观测系统和差分吸收激光雷达,分析近地面、高空φ(O₃)时空分布特征,并将φ(O₃)与温度、风速及风向3个气象要素进行相关分析. 结果表明:近地面φ(O₃)日变化明显,06:00左右为低谷,下午14:00左右达到峰值. 高空φ(O₃)的空间分布很不均匀,上层气流易使O₃富集层向下输送造成污染,同时稳定边界层对大气扩散的不利影响也是形成O₃污染的重要原因. φ(O₃)的日变化趋势与温度的日变化趋势呈显著正相关,R(相关系数)为0.74;上下层湍流交换使风速与近地面φ(O₃)呈正相关,而水平扩散使二者呈负相关;通过分析风向的分布规律发现,东北风易造成北京地区O₃污染.      

嘉兴夏季臭氧污染的近地层垂直变化特征

基于2018年浙江省嘉兴市14个环境国控站点的O₃历史资料与气象要素,研究O₃与气象要素的关系,并结合差分吸收臭氧雷达的垂直臭氧探测资料,分析近地层O₃廓线变化特征.结果表明,嘉兴地区发生高浓度O₃污染的关键气象要素为24~36℃的大气温度和36%~77%的相对湿度,24℃以上的大气温度与77%以下的相对湿度可作为启动预警O₃污染的气象指标.差分吸收臭氧雷达监测结果显示,无论O₃超标天与清洁天,在垂直方向上其浓度随高度先升后降,在600~800m范围出现峰值;O₃污染时段,在中午到午后低空形成持续向下的O₃输送带,这种低空O₃与地表O₃的叠加机制加重地表O₃污染程度,导致地表O₃超标与低空高浓度相伴出现;其廓线日变化规律表现出800m以下浓度在夜间和凌晨梯度不显著,日出后近地层O₃随时间快速增加,中午和午后持续高值,傍晚随时间逐渐下降的特征.后向轨迹分析表明,10,500,1000m高度层的气流后向轨迹聚类有相似性,500m处沿闽浙海岸线的轨迹簇对应O₃较10m处来自海上的轨迹簇高,这与500m处前体物输送堆积和紫外线辐射增强有关.污染过程近地层气流来向紧贴地面,但中高层有明显下沉气流使得O₃前体物在500m附近堆积,是造成2个典型污染过程中垂直方向上O₃高值出现在500m左右的原因之一.     

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.     

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.     

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.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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Isolation and preliminary characterization of a 3-chlorobenzoate degrading bacteria

A study was conducted to compare the diversity of 2-, 3-, and 4-chlorobenzoate degraders in two pristine soils and one contaminated sewage sludge. These samples contained strikingly different populations of mono-chlorobenzoate degraders. Although fewer cultures were isolated in the uncontaminated soils than contaminated one, the ability of microbial populations to mineralize chlorobenzoate was widespread. The 3- and 4-chlorobenzoate degraders were more diverse than the 2-chlorobenzoate degraders. One of the strains isolated from the sewage sludge was obtained. Based on its phenotype, chemotaxonomic properties and 16S rRNA gene, the organism S-7 was classified as Rhodococcus erythropolis. The strain can grow at temperature from 4 to 37℃. It can utilize several （halo）aromatic compounds. Moreover, strain S-7 can grow and use 3-chlorobenzoate as sole carbon source in a temperatures range of 10-30℃ with stoichiometric release of chloride ions. The psychrotolerant ability was significant for bioremediation in low temperature regions. Catechol and chlorocatechol 1,2-dioxygenase activities were present in cell free extracts of the strain, but no （chloro）catechol 2,3- dioxygenase activities was detected. Spectral conversion assays with extracts from R. erythropolis S-7 showed accumulation of a compound with a similar UV spectrum as chloro-cis,cis-muconate from 3-chlorobenzoate. On the basis of these results, we proposed that S-7 degraded 3-chlorobenzoate through the modified ortho-cleave pathway.     

Single and joint effects of pesticides and mercury on soil urease

The influence of two pesticides including chlorimuron-ethyl and furadan and mercury （Hg） on urease activity in 4 soils （meadow burozem and phaeozem） was investigated. The soils were exposed to various concentrations of the two pesticides and Hg individually and simultaneously. Results showed that there was a close relationship between urease activity and organic matter content in soil. Chlorimuron-ethyl and furadan could both activate urease in the 4 soils. The maximum increment of urease activity by chlorimuronethyl was up to 14%-18%. There was almost an equal increase （up to 13%-21%） in the urease activity by furadan. On the contrary, Hg markedly inhibited soil urease activity. A logarithmic equation was used to describe the relationship （P〈0.05） between the concentration of Hg and the activity of soil urease in the 4 tested soils. Semi-effect dose （ED50） values by the stress of Hg based on the inhibition of soil urease in the 4 soils were 88, 5.5, 24 and 20 mg/kg, respectively, according to the calculation of the corresponding equations. The interactive effect of chlorimuron-ethyl or furadan with metal Hg on soil urease was mainly synergic at the highest tested concentrations.     

Organochlorine pesticides in soils under different land usage in the Taihu Lake region, China

A field study was conducted in the Taihu Lake region, China in 2004 to reveal the organochlorine pesticide concentrations in soils after the ban of these substances in the year 1983. Thirteen organochlorine pesticides (OCPs) were analyzed in soils from paddy field, tree land and fallow land. Total organochlorine pesticide residues were higher in agricultural soils than in uncultivated fallow land soils. Among all the pesticides, ΣDDX (DDD, DDE and DDT) had the highest concentration for all the soil samples, ranging from 3.10 ng/g to 166.55 ng/g with a mean value of 57.04 ng/g and followed by ΣHCH, ranging from 0.73 ng/g to 60.97 ng/g with a mean value of 24.06 ng/g. Dieldrin, endrin, HCB and α-endosulfan were also found in soils with less than 15 ng/g. Ratios of p,p'-(DDD DDE)/DDT in soils under three land usages were: paddy field ＞ tree land ＞ fallow land, indicating that land usage inlfuenced the degradation of DDT in soils. Ratios of p,p'-(DDD DDE)/DDT ＞1, showing aged residues of DDTs in soils of the Taihu Lake region. The results were discussed with data from a former study that showed very low actual concentrations of HCH and DDT in soils in the Taihu Lake region, but according to the chemical half-lives and their concentrations in soils in 1980s, the concentration of DDT in soils seemed to be underestimated. In any case our data show that the ban on the use of HCH and DDT resulted in a tremendous reduction of these pesticide residues in soils, but there are still high amounts of pesticide residues in soils, which need more remediation processes.     

Alterations of organ histopathology and metallolhionein mRNA expression in silver barb, Puntius gonionotus during subchronic cadmium exposure

Common silver barb,Puntius gonionotus,exposed to the nominal concentration of 0.06 mg/L Cd for 60 d,were assessed for histopathological alterations(gills,liver and kidney),metal accumulation,and metallothionein(MT)mRNA expression.Fish exhibited pathological symptoms such as hypertrophy and hyperplasia of primary and secondary gill lamellae,vacuolization in hepatocytes,and prominent tubular and glomerular damage in the kidney.In addition,kidney accumulated the highest content of cadmium,more than gills and liver.Expression of MT mRNA was increased in both liver and kidney of treated fish.Hepatic MT levels remained high after fish were removed to Cd-free water.In contrast,MT expression in kidney was peaked after 28 d of treatment and drastically dropped when fish were removed to Cd-free water.The high concentrations of Cd in hepatic tissues indicated an accumulation site or permanent damage on this tissue.