北京城区臭氧日变化特征及与前体物的相关性分析

对2012年12月至2013年11月北京城区12个自动空气监测子站的臭氧及其前体物的浓度进行了分析,探讨北京城区臭氧浓度的日变化特征以及与前体物的关系.研究发现,北京市城区臭氧在5~8月份维持相对较高浓度,其他月份则较低.臭氧浓度呈现单峰型分布,基本在15:00、16:00达到峰值;同时臭氧呈现较明显的“周末效应”,即周末臭氧浓度高于工作日浓度. CO、NO、NO2和NOx等前体物多呈现双峰型分布,与O3均呈显著的负相关性,相关性在夏季较低.通过大气氧化剂OX和NOx的拟合方程发现,冬季北京市城区OX在白天受区域O3影响相对较大,在夜间受局地NOx污染影响相对较大.计算了在理想情况下的城区NO2光解速率,春季、夏季、秋季和冬季的平均值分别为0.180,0.209,0.169,0.149min-1.在白天臭氧的高浓度时段城区O3、NO和NO2体现出近似光化学平衡态的特征.     

基于环流分型法的地面臭氧预测模型

利用2011~2016年地面臭氧观测数据和同期地面气象要素观测及大尺度再分析资料,选取日最大8h臭氧浓度指标,分析臭氧浓度,局地气象要素以及大尺度环流因子的关系,并将Lamb-Jenkinson客观环流分析方法与逐步回归模型结合,建立臭氧浓度逐日预报模型.结果表明,杭州地面臭氧浓度呈季节性变化特征,春夏两季杭州臭氧平均浓度较高,为臭氧超标易发时段,其中5月臭氧浓度超标频次最高.地面臭氧浓度受局地气象要素影响显著,其中总辐射和日最高气温与臭氧浓度呈显著正相关,相对湿度和降水则呈负相关.在客观分型得到的10种环流型中,杭州全年受反气旋环流控制的概率最高,占26.5%,受西北气流环流控制的概率最低,仅占0.6%.在南风型环流形势下,杭州臭氧浓度超标频率最高,达23.8%,北风型环流形势下的臭氧浓度超标频率最低,为3.7%.基于季节环流分型的地面臭氧预报模型对预报效果改进明显,2016年模型预报值与观测臭氧浓度值相关系数达到0.87.模型尤其提高了高浓度臭氧事件预报准确性,2016年共24次臭氧超标事件,模型成功预报15次,TS评分达到52%.     

昆明市臭氧污染特征及与气象因子关系初步研究

对昆明市2014—2018年空气质量和臭氧(O3)污染特征进行了分析,并结合臭氧污染观测资料和气象条件,对昆明市臭氧浓度与气象因子相关性进行了初步研究。结果表明:昆明市空气质量总体逐渐变好,臭氧浓度整体呈上升趋势,春季和夏季臭氧污染比较明显;臭氧浓度春季高,秋冬季低,高值主要集中在3—5月;臭氧污染主要出现在3—8月,7月最高;臭氧浓度与太阳辐射、气温、大气低层温度垂直分布、风速等总体呈正相关,与气压、相对湿度总体呈负相关。     

西安城区夏季地面臭氧浓度变化特征分析

于2013年夏季,对西安城区10个大气监测点进行了地面大气中O3及其前体物(NOx、CO)连续在线观测,观测结果分析表明:夏季O3小时浓度平均值范围为39.03~93.06μg/m3,且其浓度呈现由东北至西南方向逐渐升高的空间分布特征。O3小时浓度分布呈明显的单峰形式,15:00左右达到峰值;NOx、CO浓度呈较明显的双峰分布,CO较NOx的浓度波动较为平缓。O3日均浓度与温度、太阳辐射呈正相关,而与相对湿度呈负相关关系,且受温度、太阳辐射的影响更加显著。     

北京地面紫外辐射与空气污染的关系研究

基于北京城区太阳辐射和污染气体观测资料,运用TUV4.4辐射传输模型,研究了城市大气中太阳紫外辐射与空气污染的相互关系.结果表明,臭氧总量平均为329DU,并呈冬春季较高,夏秋季较低的季节变化规律,到达地面的紫外辐射呈现相反的变化趋势;受城区大气污染的影响,地面处的紫外辐射量大幅减少(最大50%),且在夏季波动较大;云和污染物对紫外辐射的影响要大于总辐射,紫外辐射衰减约为总辐射衰减的2倍;城市低层大气中O3和NOx浓度的增加是造成紫外辐射衰减的重要原因,午后O3浓度与紫外辐射衰减相关系数为0.70.     

常州地区近地面O3及其前物体相关性研究

根据2013年全年至2014年6月常州市环境监测中心空气自动监测系统监测子站的臭氧(O3)及其前体物(氮氧化物NOx和一氧化碳CO)的数据资料,着重分析了上述监测因子时间变化特征,并研究了三者之间的相关性.结果表明,受局地光化学反应,常州地区在冬夏两季O3污染程度相差较大,夏季为O3的活跃期浓度较高.O3单日浓度呈单峰型变化.NOx和O3浓度基本成正相关.CO的浓度变化与O3的浓度变化呈明显的正相关,且CO污染相对于O3污染有明显的滞后性.     

基于PSCF与CWT模型对乌鲁木齐市地表臭氧源区分析

乌鲁木齐市是中国西部典型的重工业城市,伴随着快速的工业化和城市化发展,城市大气臭氧污染日益严重。为探究乌鲁木齐市地表臭氧污染特征,该研究采用2015-2019年乌鲁木齐市大气污染物监测数据及同期气象观测资料,结合统计分析、后向轨迹分析、潜在源贡献因子以及浓度权重轨迹对乌鲁木齐市臭氧污染特征及潜在源区进行分析。结果显示,(1)2015-2019年乌鲁木齐市臭氧年评价指标由118μg/m³增长至128μg/m³。同时,乌鲁木齐市主要大气污染正经历由颗粒物向臭氧过渡的变化,其作为首要污染物占比从2015年的5.8%上升至2019年的28.0%,不同季节臭氧浓度变化特征为夏季>春季>秋季>冬季,且在分布特征上与NO₂、CO呈显著负相关。(2)后向轨迹分析结果表明：影响乌鲁木齐市大气臭氧分布的气流具有途经境外地区、长距离迁移、高浓度的特征,境内气流迁移途径普遍较短且对乌鲁木齐市臭氧浓度传输影响较小。(3)潜在源贡献因子法与浓度权重轨迹法表明,影响乌鲁木齐市臭氧浓度的主要源区与贡献高值区是昌吉州、塔城地区、博尔塔拉...     

2015～2018年太原市臭氧污染特征分析

基于太原市2015年1月~2019年2月的空气质量监测数据,分析了太原市近地面臭氧浓度变化特征。结果表明:2015~2018年太原市臭氧年平均浓度为78.42、82.33、95.87、103.77μg/m 3,臭氧浓度存在加速上升趋势;臭氧浓度逐日变化范围为5~270μg/m 3,共有181 d超过GB 3095—2012《环境空气质量标准》二级标准限值(160μg/m 3),超标时段主要集中于5~8月份;臭氧浓度日变化呈单峰型分布,峰值与谷值时段分别为14∶00~16∶00和6∶00~7∶00;臭氧浓度有明显的月变化规律,峰值与谷值时段分别为6~7月和1月、12月;臭氧浓度还表现出显著的季节变化规律,按浓度高低依次排序为夏季、春季、秋季和冬季;臭氧浓度与NO 2、CO、PM 2.5浓度呈负相关性。     

人为源和生物源排放对臭氧的贡献 ——以春夏季东亚地区为例

利用因子分离法区分NOx与人为、生物源VOCs(AVOCs、BVOCs)分别对东亚地区近地面O3浓度的纯贡献与协同贡献,基于区域空气质量模式(RAQM)讨论了2000年春、夏季排放源的总贡献以及协同贡献的空间分布.结果表明,光化学反应在日最大O3浓度的形成中占很大比例,我国北方大部分地区源的贡献夏季最大,南方受东亚季风影响,夏季最小.AVOCs与NOx、BVOCs与NOx的协同效应加强了光化学反应中O3的形成.AVOCs与NOx的协同贡献季节性变化特征显著,我国南方大部分地区夏季最小.BVOCs与NOx的协同贡献在我国南北方差异很大,春季高值区主要分布在南方大部分地区,北方峰值出现在夏季.说明臭氧调控对策的制定除源排放大小外还须考虑地域差异和季节变化.     

粤东北地区臭氧与前体物关系

选取梅州为粤东北地区代表城市,使用高阶去耦合直接法(High-order Decoupled Direct Method,HDDM)开展臭氧与前体物关系研究。一阶敏感性系数表明,在夏季,减少省外VOCs或NOx排放对梅州的臭氧污染控制都有利,梅州本地VOC排放的减少有利于降低臭氧浓度,但NOx的减排反而会加重臭氧污染水平,而省内其它城市排放的变化在大部分时候对梅州影响轻微。秋季,梅州本地的排放对梅州的臭氧影响最大,其次是外省的排放,广东省其它城市的影响轻微,减少省外或梅州市本地VOCs排放对梅州的臭氧污染控制都有利,省外NOx排放的减少在个别时候有利于降低臭氧浓度,个别时候会加重梅州臭氧污染,但梅州本地NOx的减排会加重臭氧污染水平。考虑二阶敏感性系数的臭氧与前体物排放变化曲线表明,粤东北地区的臭氧与外省前体物的排放或广东省其它城市前体物的排放呈现出高度的非线性关系。而梅州本地臭氧前体物的排放变化与臭氧浓度变化的关系较为线性。建议粤东北地区尽可能减少本地排放的VOCs以减轻臭氧的污染水平。     

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.