某钢厂大气PM_(2.5)污染特征与潜在源区贡献分析

基于2017年全年在某钢厂厂区4个特征点位进行的环境大气PM_(2.5)、PM_(10)和气象参数的在线监测数据,对一年中污染高发/非高发时段钢铁厂厂区内大气颗粒物的浓度水平、粒径分布、日均值变化趋势以及气象因素对浓度的影响进行了分析,并利用大气气团输送模拟及潜在污染源贡献(PSCF)分析探讨了厂区大气PM_(2.5)的外来输送和本地贡献情况。结果表明:2017年全年某钢厂厂区大气颗粒物以细颗粒物为主;4个站点大气PM_(2.5)日均值全年变化趋势一致,污染高发月份质量浓度均值高于非污染高发月份相应值;除2号站可能受到厂区生产活动排放的影响,PM_(2.5)浓度水平略高外,各站点相互间及与周边环境对照点的浓度保持在一致水平,亦未发现明显的污染物输出现象;冬季外来污染源输入对厂区大气PM_(2.5)浓度贡献较显著,其他季节应主要考虑本地排放影响。     

北京市大气环境PM2.5和PM1及其碳质组分季节变化特征及来源分析

大气颗粒物是影响我国大多数城市环境空气质量的首要污染物,近年来随着监测技术的进步和采样设备的改进,相关研究对象逐渐从大粒径的PM_10、PM_(2.5)转移到更小粒径的PM_1上.碳质组分是大气颗粒物的重要组成部分.以北京市为研究区域,选取2016年7月、10月及2017年1月、4月作为4个季节的代表月,对大气环境中的PM_(2.5)和PM_1进行采集,分析了二者的质量浓度和季节变化特征.采用两层嵌套气象-空气质量模型系统(WRF-CMAQ)耦合模型对采样时段进行了模拟,分析观测期间PM_(2.5)和PM_1的来源贡献,并使用因子分析法解析了碳质组分的来源.结果表明,PM_(2.5)和PM_1的质量浓度均呈现春、夏、秋、冬这4个季节递增的趋势;PM_1是PM_(2.5)中的主要组成,而且秋冬季节随着灰霾发生频率的增加,PM_1质量浓度占PM_(2.5)的比值明显升高;北京市大气环境中存在明显的二次污染,且SOC更容易在粒径更小的PM_1中积聚.散煤燃烧、机动车尾气排放、居民面源及生物质燃烧排放是北京市大气颗粒物的重要贡献来源;汽油车尾气、柴油车尾气、生物质燃烧和燃煤排放是北京市大气颗粒物中碳质组分的主要来源.     

基于本地污染源调查的杭州市大气污染物排放清单研究

基于实地调查数据并辅以统计数据,采用物料衡算法和排放因子法,估算了杭州市2015年大气污染物排放清单,并选取经纬度坐标、路网、航道、土地类型和人口等数据作为权重因子,研究了该地区各类排放源污染物排放空间分布特征.结果表明,杭州市2015年SO_2、NO_x、CO、VOCs、PM_(10)、PM_(2.5)和NH_3年排放总量分别为22.20×10~3、108.17×10~3、192.10×10~3、134.94×10~3、78.12×10~3、27.65×10~3和59.75×10~3t.工业源是杭州市SO_2排放的主要来源,移动源对NO_x和CO的排放贡献最为显著,扬尘源是杭州市PM_(10)和PM_(2.5)排放的最主要来源,其次为工业源;VOCs排放的主要来源依次为工业源、天然源和移动源;NH_3排放主要来自农业源.从空间分布来看,排放主要集中在中心城区及其周边的萧山、下沙、大江东、余杭和富阳等工业企业相对密集的区域.本研究建立的排放清单在污染源覆盖范围和排放因子方面仍然存在一定的不确定性,建议在后续研究中重点开展低、小、散企业及本地化排放因子调查研究工作,进一步提升大气污染物排放清单的准确度.     

温州城区大气污染特征数值模拟与来源解析

文章以位于温州城区的瓯海区为例,在建立大气污染源清单的基础上,利用WRF-CMAQ、CALPUFF模型分析了外来污染物区域输送对瓯海区的影响,模拟了瓯海区主要大气污染物浓度分布,解析了区域大气污染物排放来源。WRF-CMAQ模型模拟结果表明,区域大气污染物SO_2、NO_2、PM_(10)和PM_(2.5)的输送对瓯海区的贡献影响均呈现冬季(1月)>春季(4月)>秋季(10月)>夏季(7月)的变化规律,这可能与大气污染物来源有关。CALPUFF模型模拟结果显示,瓯海区SO_2和PM_(10)的年平均浓度达标,但NO_2和PM_(2.5)出现超标现象。除SO_2均能达标外,部分敏感目标处NO_2、PM_(10)和PM_(2.5)年平均浓度有不同程度的超标现象。来源分析结果表明,瓯海区大气污染物SO_2和NO_2主要来自本地源排放,而PM_(10)和PM_(2.5)本地源与外来源的排放贡献相当。     

恩施州大气污染物排放量估算及清单构建

该文通过污染源现场调查和部门资料收集,结合全国第二次污染源普查和湖北省污染源自动监控综合管理系统,以2017年为基准年,对恩施州大气污染物排放量进行了估算,并建立了恩施州1 km×1 km大气污染源排放清单,研究分析了清单结果和普查结果的差异。结果显示,2017年恩施州人为源SO_2、NO_x、CO、VOCs、PM_(10)、PM_(2.5)、BC、OC和NH_3排放总量分别为12 702.26、19 610.04、168 721.49、16 709.92、17 382.89、10 789.67、3 593.30、5 848.86和43 778.37 t;天然源挥发性有机物(BVOCs)排放总量为159 239.47 t。其中,固定燃烧源是SO_2、CO、PM_(10)、PM_(2.5)、BC和OC主要来源,移动源是NO_x和VOCs的主要来源,NH_3的主要来源是农业源,PM_(10)、PM_(2.5)排放主要来自扬尘源。阔叶林和针叶阔叶混交林对天然源排放贡献较大。空间分布上,污染物排放主要集中在恩施市、利川市和巴东县。对比清单结果和普查结果,SO_2和VOCs排放量估算较普查结果高,NO_x排放量估算与普查结果相差不大。     

中国国道和省道机动车尾气排放特征

近年来,随着我国机动车保有量的持续增长,机动车排放已成为我国重要的大气污染物来源之一.现有的机动车排放研究多关注城市内的机动车大气污染物排放,针对城市间的大气污染物排放研究较少.我国城市间交通道路主要包括国道和省道,截止至2015年我国国道里程18.53万km、省道里程32.97万km,约占全国等级公路总里程的13%,因此开展我国国道和省道机动车大气污染物排放研究十分重要.本研究基于全国国道和省道交通监测站的年均监测数据,采用环境保护部发布的《道路机动车大气污染物排放清单编制技术指南(试行)》中的指导方法,计算了2015年我国国道和省道机动车的大气污染物排放清单,分析了污染物排放的时空分布特征.结果表明,我国国道和省道公路机动车排放的一氧化碳(CO)、氮氧化物(NO_x)、颗粒物(PM)和碳氢化合物(HC)排放量分别占全国机动车污染物总排放量的4.5%、27.9%、14.4%和7.7%;不同车型对国道和省道机动车大气污染物排放的分担率不同,其中大货车是NO_x、PM_(10)、PM_(2.5)的主要来源,摩托车是CO和HC的主要来源;不同道路类型中各车型的大气污染物排放分担率也不同,如高速路上大货车是NO_x、PM_(10)和PM_(2.5)的主要来源,普通道路上大客车和大货车是NO_x、PM_(10)和PM_(2.5)的主要来源.     

大气污染物和污染源重要性排序研究

为了在现有大气污染源排放清单建设工作中突出重点,进行有效的调研分析,需判断出区域大气的主要污染源和污染物,因此制定了区域大气污染物和污染源重要性排序的一般原则和计算方法。从现有国内研究中选取北京市、天津市、上海市、杭州市、广东省以及珠三角共6个有NO_x、SO_2、PM_(2.5)、PM_(10)、NH_3、VOCs、CO排放量研究结果的地区进行综合对比分析,根据等标污染负荷比法和狄克松检验法得出区域污染源和污染物重要性排序结果。根据通用方法,以扬州市为例,得出扬州市大气污染源重要性排序结果依次为:工业源、生活源、农业源、移动源和其他源,主要污染源为工业源和生活源;扬州市大气污染物重要性排序结果依次为:NO_x、SO_2、PM_(2.5)、PM_(10)、NH_3、VOCs和CO,主要污染物为NO_x、SO_2、PM_(2.5)和PM_(10)。     

南宁市生物质锅炉排放的颗粒物中碳组分特征

针对生物质锅炉排放的颗粒物,分别采集了PM_(10)和PM_(2.5),主要研究了颗粒物中碳组分特征、粒径分布等.采用热光反射法(TOR)测定了样品中的有机碳(OC)和元素碳(EC)含量,得到char-EC和soot-EC的含量.结果表明,不同的除尘方式对生物质锅炉排放颗粒物中的OC和EC含量有明显的影响;作为识别源的指标OC/EC值和chart-EC/soot-EC,测得布袋除尘样品中,OC/EC和char-EC/soot-EC在PM_(10)中分别为1.4±0.4和35.7±16.5,在PM_(2.5)中分别为2.2±1.3和15.5±10.3;旋风除尘PM_(10)样品中OC/EC值和char-EC/soot-EC分别为6.1±1.9和5.2±2.5,旋风除尘PM_(2.5)样品中6.5±2.0、2.5±2.3.对8个碳丰度分析可知,布袋除尘样品中EC1在TC中的占比最高;旋风除尘样品中OC1-OC3在TC中占比较高.此外,OC2、OC3和EC2主要富集在PM_(2.5)中,OC4、EC1和EC3主要富集在PM_(10)中.     

供热锅炉颗粒物排放特征实测研究

采用芬兰Dekati公司的颗粒物稀释采集系统对天津市供热行业7台典型燃煤锅炉、1台天然气锅炉开展PM_(10)、PM_(2.5)排放特征实测研究,结果表明:(1)燃煤锅炉在湿法除尘和旋风除尘器后的PM_(10)、PM_(2.5)排放因子具有显著差异(湿法除尘:PM_(10)(0.341±0.289)kg/t、PM_(2.5)(0.305±0.270)kg/t;旋风除尘:PM_(10)(0.608±0.163)kg/t、PM_(2.5)(0.558±0.165)kg/t);燃气锅炉PM_(10)、PM_(2.5)排放因子均为0.025kg/万m~3,其测试结果与国内已有研究结果具有很好的可比性。(2)燃煤锅炉PM_(10)、PM_(2.5)排放因子实测值显著低于物料衡算法,说明采用物料衡算法对清单中一次颗粒物的排放量估算存在高估的可能性。(3)供暖锅炉污染物排放存在显著的时间变化特征,清晨与午后分别是排放量高峰和低谷时间段。     

典型道路路边空气颗粒物及无机元素特征分析

于2015年春、夏季,在天津市选取4条不同等级道路进行路边空气颗粒物(PM_(2.5)和PM_(10))采集,并分析其中16种无机元素.结果表明,春季PM_(2.5)和PM_(10)的平均浓度显著高于夏季.路边环境中PM_(2.5)/PM_(10)低于非路边环境中空气颗粒物比值,且次干道和快速路分别在PM_(2.5)和PM_(10)中污染最严重.元素浓度分析显示,PM_(2.5)和PM_(10)中Si、Al、Ca等地壳元素浓度最高,次干道和快速路受人为元素影响较大,外环路所受影响较小;富集因子(PM_(2.5)和PM_(10))分析结果显示,Pb、Zn、Cu、Sb、Sn和Cd的EF10,是路边环境中富集程度较高的元素.通过Kruskal-Wallis H检验,PM_(2.5)中各元素富集因子在4条道路上存在显著性差异,次干道受机动车污染较严重.PM_(2.5)和PM_(10)中因子分析结果有一定差异,PM_(2.5)分析结果显示采样期间该区域主要污染源有开放源(土壤尘、扬尘、道路尘及建筑尘)、机动车排放源(尾气和非尾气源)、燃烧源和工业源,其中机动车排放源在人为源污染中占比最高.     

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.