2017—2020年前体物与气象因子对承德市臭氧污染的影响

利用2017—2020年承德市环境监测站和承德市国家基准气象站的数据,分析了承德市近地层O3浓度特征,O3与其他污染物之间的关系和气象因子对O3浓度的影响.结果表明,2017—2020年承德市年平均O3超标日数40天,占总超标日数的55％.承德市O3-8h浓度呈现夏季>春季>秋季>冬季的季节变化特征,5—7月份O3-8h浓度最高,平均浓度超过160μg·m-3.O3浓度的日变化表现为单峰型分布,O3浓度最低值出现在清晨7:00—8:00时,峰值出现在14:00—16:00时.O3-8h浓度与细颗粒物PM10和PM2.5在夏季呈显著的正相关关系,其他季节相关性不显著;O3-8h浓度与前体物CO和NO2在夏季呈显著的正相关关系,冬季呈显著的负相关关系.太阳总辐射强度大于750 W·m-2,最高气温大于30℃,无降水和相对湿度30％～60％,受地面偏南气流影响的气象条件下,承德市易于出现O3-8 h浓度超标天气.     

许昌市臭氧污染趋势及时空分布特征研究

为研究许昌市的臭氧(O3)污染情况及时空分布特征,对2014年-2016年许昌市3个国家环境空气监测点位的监测数据进行了统计分析.结果表明:2014年-2016年,许昌市O3污染状况整体呈加重趋势,2016年污染最为严重;O3浓度和超标天数均具有明显的季节变化特征,春末和夏季的O3污染最为严重;不同季节的O3、NO2、NO和NOx浓度日变化也不尽相同,同时O3具有明显的日变化特征,呈单峰型分布,峰值出现在14:00~15:00;并且O3与NO2具有较好的相关性.     

杭州市近地面大气臭氧浓度变化特征分析

利用2012~2016年杭州市近地面臭氧(O_3)的连续观测资料以及气象数据,分析了杭州市近地面O_3浓度的变化特征及其与气象要素的关系.结果表明,近年来杭州市O_3年平均浓度较10年前升高10μg/m~3左右,光化学污染形势日趋严重.O_3浓度冬季较低,其余季节均较高,日平均浓度大于100pg/m~3主要分布在4~10月.O_3浓度日变化呈单峰型分布,5:00~7:00出现最低值,14:00出现峰值,超标时段主要出现在11:00~18:00.O_3浓度变化与紫外辐射、温度呈正相关关系,与相对湿度呈负相关关系.紫外辐射大于0.02MJ/m~2、气温高于20℃、相对湿度低于70%时,O_3浓度会出现超标情况.风向风速对O_3浓度有一定影响,当风向为北风或偏北风时,O_3浓度较低;当风向为东风或偏东风时,O_3浓度较高,说明影响杭州O_3浓度升高的污染源也主要来自东部,南部和北部地区较少.     

重庆市北碚城区大气污染物浓度变化特征观测研究

为了研究重庆市北碚区大气污染物浓度变化特征及其污染状况,采用全自动在线监测仪器对重庆市北碚城区大气污染物进行连续在线监测,分析了2012年1月~2013年2月的大气污染物观测数据.结果表明,除SO2以外,其它污染物均有超出国家新环境空气质量标准(GB 3095-2012)的情况出现,其中细粒子污染最严重.大气污染物浓度具有明显的季节变化,2012年春夏秋冬季各污染物平均浓度:O3为(36.1±19.2)、(48.8±32.6)、(29.8±28.6)、(18.2±15.8)μg·m-3,Ox为(77.6±20.6)、(91.3±37.6)、(77.5±30.6)、(69.4±18.2)μg·m-3,表现为夏高冬低;NO为(11.8±9.4)、(8.2±4.9)、(20.7±17.1)、(30.4±25.1)μg·m-3,NO2为(42.3±13.1)、(40.5±9.9)、(47.2±14.1)、(51.2±15.9)μg·m-3,NOx为(54.1±20.8)、(48.7±12.6)、(67.9±25.5)、(81.6±37.9)μg·m-3,均表现为冬高夏低;SO2为(50.5±23.3)、(26.3±16.7)、(38.8±18.4)、(53.7±23.4)μg·m-3,表现为冬春高而夏秋低;而PM2.5则为(61.4±28.5)、(68.1±32.5)、(61.9±27.1)、(89.6±44.2)μg·m-3,表现出冬季高而其它季节比较平稳的特征.O3、Ox、NO、NOx以及SO2浓度均为单峰型的日变化形式,其中O3和Ox的日变化峰值出现在午后16:00,而NO、NOx及SO2的日最大值则出现在08:00~11:00;NO2和PM2.5的日变化模态呈双峰型,有早晚两个峰值.O3和Ox在夏季日变化振幅最大,而其它污染物则冬季日变化振幅最大.将工作日与周末各污染物浓度的日变化相比,成对t检验分析表明,NO并无明显差异(P=0.14),但N2O工作日显著高于周末(P=0.03),而O3则为工作日极显著低于周末(P<0.001).相关分析表明,O3浓度与气温和风速呈显著或极显著正相关,与相对湿度呈极显著负相关,而NOx则与以上各气象要素的关系正好相反;PM2.5与气温和风速呈负相关,与相对湿度呈正相关;SO2与各气象要素的关系在不同的季节表现不同.除此之外,风向也是影响大气污染物浓度的一个重要因素.     

广州近地面臭氧浓度特征及气象影响分析

利用2015年广州市近地面逐时臭氧(O_3)观测资料及气象数据,分析了广州地区近地面的O_3浓度时空分布特征及其与气象因子的关系.结果表明:广州地区城郊的O_3浓度高于中心城区;广州地区近地面的O_3浓度超标时间主要出现在4—9月,8月O_3浓度最高,3月O_3浓度最低;O_3浓度日变化呈现"单峰型"分布,早上7:00—8:00出现最低值,15:00达到峰值;O_3浓度与气温呈正相关,当气温高于30℃时,O_3浓度随温度升高增加明显;与相对湿度呈负相关,当相对湿度大于60%时,O_3浓度显著降低;当气压小于1010 hpa时,与气压呈负相关,当气压大于1010 hpa时,与气压呈正相关;当风力为2~3级吹西北偏西至西南偏西风区间时,O_3浓度最高,说明广州偏西部可能存在O_3污染源区;O_3浓度在晴天最高,其次是少云和多云天气,最低是在雨天.总体而言,气温高、日照长、辐射强、气压低、湿度小及2~3级的风力是广州地区近地面产生高浓度O_3的主要气象因素.当广州O_3浓度出现超标时,气温变化范围为25.9~37.4℃,相对湿度变化范围为29%~83%,气压变化范围为989.4~1009.1 h Pa,风速变化范围为0.7~5.8 m·s~(-1),紫外辐射强度日最大1 h均值最小为32.6 W·m~(-2),10:00—14:00均值最小为27.3 W·m~(-2).     

成都市大气中挥发性有机物的时空分布特征及臭氧生成潜势研究

对成都市2011—2012年期间大气中的VOCs在不同季节、不同功能区及不同高度的浓度和组成进行了SUMMA钢罐采样法监测与实验室分析,并讨论其臭氧生成潜势.结果表明:采样期间成都市大气中VOCs的季节变化为:秋季(106.0μg·m-3)夏季(74.5μg·m-3)春季(54.1μg·m-3)冬季(45.8μg·m-3).烷烃、酯类、醇类日变化规律呈单峰型,峰值在8:00出现,与交通流量的变化有关;烯烃和芳香烃的日变化规律则呈双峰型.烷烃、烯烃、芳香烃、醇类在不同功能区的浓度顺序为:交通居民混合区工业区风景区,而醛酮类则为:工业区交通居民混合区风景区.在垂直方向上,距地面78 m处TVOCs浓度最高,这可能与当时采样期间大气为逆温层结有关,其中,烷烃、芳香烃为主要组分.不同VOCs的平均臭氧生成潜势(OFP)及其贡献率排序为:芳香烃(75.5%)烯烃(23.8%)烷烃(0.8%);不同功能区的OFP排序为:交通居民混合区工业区风景区.     

沈阳市挥发性有机物污染特征及反应活性

2019年对沈阳市大气挥发性有机物(VOCs)开展了为期l a的观测,并对得到的53种物种进行浓度特征以及反应活性的研究.结果表明,观测期间沈阳市VOCs平均浓度为65.33 μg·m-3,烷烃、烯烃和芳香烃质量分数分别为62.44％、16.52％和19.32％.浓度排名前10的物种主要是C3～C5的烷烃、烯烃和部分芳香烃,累计占VOCs总浓度的64.13％.大气中烷烃、烯烃和芳香烃浓度均表现为双峰型的日变化特征,峰值分别出现在06:00～08:00和19:00～20:00,最低点出现在14:00～15:00;月变化上,该地ρ(VOCs)分别在12月和5月达到最高值(136.44μg.m-3)和最低值(35.61 μg·m-3);VOCs表现出明显的季节变化特征,即冬季＞秋季＞夏季＞春季,且烷烃、烯烃和芳香烃均随季节表现出增加趋势.通过特征值甲苯/苯(T/B)研究发现,沈阳春季VOCs主要来源于交通源和采暖源,夏季主要来源机动车尾气以及溶剂挥发,秋冬季主要受生物质燃烧和煤燃烧等排放源的影响.通过对反应活性分析,燃烧源是沈阳市控制臭氧污染的关键,丙烯、乙烯和1-己烯是沈阳市大气VOCs中反应活性最高的物种.     

北京市大气中CO的浓度变化监测分析

CO是城市大气中一种重要的污染物,在城市和区域的光化学反应中起着重要的作用.用装配氢火焰离子化检测器(FID)的HP5890II气相色谱(GC)方法,以每10min的采样频率,在北京中科院大气物理研究所325m气象环境观测铁塔上(39°9′N,116°4′E),对北京城市大气CO浓度进行了连续监测,时间为2004-01～2004-12.结果显示北京城市大气CO浓度日变化呈双峰型,1d之中出现2个高峰期,早晨07:00～08:00和夜晚22:00～23:00,最高浓度值分别达到13.8mg·m-3,17.1mg·m-3.不同季节CO的日变化存在差异:冬季、秋季的日变化幅度大,而夏季、春季的日变化幅度小.秋季、冬季早晨上班高峰期后CO浓度下降快,春季、夏季上班高峰期后CO浓度下降慢.CO的这种日变化是由地表排放源和气象条件共同决定的.另外,CO存在明显的季节变化,总的表现为浓度最高值出现在冬季12月份(4.0±3.4)mg·m-3,浓度最低值出现在5月份(1.7±0.7)mg·m-3.整个观测期间1a的平均浓度为(2.6±1.9)mg·m-3,采暖期平均浓度为(3.5±2.6)mg·m-3,非采暖期平均浓度为(2.2±1.2)mg·m-3.     

北京城区和郊区本底站大气污染物浓度的多时间尺度变化特征

利用北京城区海淀宝联站(HD)和上甸子本底站(SDZ)2005—2012连续8年的大气污染物(PM_(2.5)、O3、NO2、SO_2和CO)浓度观测数据进行统计分析,揭示北京城区和郊区主要污染物浓度变化特征、超标情况及其差异.主要结论如下:1连续8年北京城区、郊区PM_(2.5)浓度整体呈缓慢下降趋势,但污染水平仍较高.海淀宝联站和上甸子本底站的PM_(2.5)年均浓度从奥运前3年(2005—2007)的平均值87.1μg·m-3和53.4μg·m-3分别下降到奥运后5年(2008—2012)的平均值67.7μg·m-3和42.1μg·m-3.奥运后5年两站PM_(2.5)年均浓度变化不大,其中城区维持在66~70μg·m-3的高浓度水平.城区PM_(2.5)浓度为3级以上的超标日在四季的发生频率相当,4级和5级以上的超标日则多发生在秋、冬季;各季平均日变化趋势均为双峰双谷型,上下班交通高峰期对PM_(2.5)浓度日变化有重要影响.2城区站O3年均浓度前5年(2006—2010)逐年下降,之后浓度开始回升,而本底站O3年均浓度在此期间变化不大,近6年(2007—2012)维持在72.4~76.3μg·m-3.城、郊O3平均日变化均呈单峰型,其中上甸子站峰值出现时刻晚于城区海淀宝联站.32005—2012年北京城区其它气态污染物浓度(NO2、SO_2和CO)总体均呈缓慢下降趋势,但在2012年浓度有所反弹,城区站气态污染物在秋、冬季的平均浓度均显著高于春、夏季.     

沈阳市O3时空分布特征及其与NOx的相关性研究

利用2013年沈阳市11个空气质量自动监测站的大气O3自动连续监测数据,对O3浓度的区域分布、季节变化、日变化及其与NOx相关性等特征进行分析.结果表明,中心城区O3浓度低于外围.O3和大气氧化性OX（O3＋NO2）浓度在午后15：00左右出现峰值,NOx呈双峰态日变化,在7：00和23：00左右出现峰值.不同季节污染物的浓度变化存在差异,O3和NOx浓度分别在夏季与冬季达到最大.NOx浓度存在200 μg/m3左右的“分界点”,NOx低于分界点时以NO2为主,高于分界点时NO占大部分.OX区域贡献主要受区域背景O3的影响,局地贡献主要受局地光化学反应制约.     

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.     

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.     

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.     

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.     

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.     

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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