中国大气气溶胶粒谱分布研究进展

大气气溶胶粒子浓度和粒径分布受不同环境和气象条件制约,分析其分布特征对研究大气环境具有重要意义。该文综合论述了近20年来中国大气气溶胶的谱分布研究进展,重点讨论了背景大气气溶胶、城市型气溶胶、海洋型气溶胶和沙尘气溶胶谱分布特征及相应的对数正态分布谱分布函数参数值,介绍了气溶胶谱分布垂直分布特征,并简述了气溶胶谱分布对大气能见度、人体健康及其对新粒子形成的影响,为大气环境相关研究以及各种气候模式提供参考。     

春节期间南京市大气气溶胶粒径分布特征

为研究春节期间燃放烟花爆竹对城市大气气溶胶数浓度粒径谱分布的影响,对2012年1月19~31日南京大气气溶胶数浓度、污染气体浓度和质量浓度进行了观测分析.结果表明,烟花爆竹的燃放期间10~20 nm气溶胶浓度远低于非燃放期,50~100、100~200和200~500 nm数浓度有较大增加,20~50 nm和0.5~10μm气溶胶数浓度变化不大.烟花爆竹的燃放对气溶胶数浓度谱影响较大,非燃放期数浓度谱为双峰型分布;在燃放期数浓度谱为单峰性分布,且峰值向大粒径段偏移.烟花爆竹燃放期间质量浓度谱为双峰型分布,对细粒子的质量浓度影响较大,燃放期间PM2.5/PM10和PM1.0/PM10的值可升高10%.烟花爆竹的大量燃放对1.0~2.1μm粒径段气溶胶密度影响最大,对其他粒径段密度影响较小.     

河北中南部不同天气条件下气溶胶的航测研究

利用粒子测量系统PMS探测的气溶胶等资料,结合观测期间的天气实况和气团后向轨迹对2008年秋季河北中南部不同天气条件下的大气气溶胶空间分布特征进行了分析和研究.结果表明:不同天气背景下河北中南部气溶胶数浓度的垂直分布和气溶胶粒子谱分布特征存在显著差异.混合层高度,逆温层和相对湿度峰值引起的气溶胶累积效应,云层分布不均以及气溶胶来源特性差异对气溶胶的空间分布特征有着重要影响.不同天气条件下河北中南部近地面的气溶胶数浓度范围为904.4~3005.0个/cm~3.近地面气溶胶数浓度阴天条件下最高,晴空条件下最低.气溶胶粒子谱分布特征与大气层结,逆温层,云区分布等密切相关.逆温层是导致粒子谱呈双峰或多峰分布的主要原因之一.由于云内气溶胶粒子吸湿增长,粒子谱峰值向大尺度方向偏移.云外的气溶胶粒子谱宽且比云内窄.受大气气溶胶粒子本身重力沉降作用的影响,高层粒子谱宽比低层窄,粒子谱峰值向小尺度方向偏移.     

大连海域大气气溶胶特征分析

本文分析和讨论了１９９４、１９９５两年在大连石槽海洋大气观测站所监测的大气气溶胶及气溶胶中元素和离子的浓度、富集程度、相互关系等物理、化学特征，还讨论了天气及某些气象要素对气溶胶浓度分布特征的影响，对气溶胶的来源也作了简要探讨。     

南京夏季清洁与污染区气溶胶微物理特征分析

为研究南京地区大气气溶胶粒子的微物理特征,于2008年8月～2008年9月在南京北郊和南京紫金山对照点进行了大气气溶胶观测,文章分析了气溶胶的浓度、谱分布、日变化特征以及降水对其数浓度的影响。结果表明:南京北郊大气气溶胶日平均数浓度约是紫金山的2.6倍,最大值数量级高达106,比紫金山高出2个量级;南京北郊气溶胶数浓度谱分布呈单峰分布,紫金山观测区呈双峰分布,峰值都集中在爱根核模态;气溶胶的表面积浓度分布集中在积聚模态,质量浓度则主要集中在积聚模态和粗粒子模态;气溶胶表现出明显的日变化,紫金山观测区上午达到全天最大值,南京北郊午后达到全天最大值,受人为活动影响较大;气溶胶的数浓度与降水强度呈负相关性,降水对粒径范围为0.02μm～0.1μm的气溶胶有很强的清除作用。     

天津冬季相对湿度对气溶胶浓度谱分布和大气能见度的影响

于2013年1月连续在线观测天津城区气溶胶数浓度谱分布和大气能见度,并结合相关气象资料,探讨相对湿度(RH)对气溶胶浓度谱分布和大气能见度的影响.结果表明,观测期间发生了4次连续雾霾天气过程, 4次雾霾天气过程对应着气溶胶粒子数浓度的连续高值,低能见度天气系高浓度气溶胶粒子和高相对湿度协同所致;随着RH增大,PN1和PN2.5-10呈增长趋势, RH>90%后,PN1和PN2.5-10有所降低,PN1-2.5则持续增长,高RH对气粒转化和气溶胶粒子的碰并聚合作用明显;气溶胶吸湿增长因子计算表明,高RH下水汽对能见度影响很大,尤其是大雾天气下其影响甚至可能超过气溶胶粒子浓度对其的影响.     

天津冬季相对湿度对气溶胶浓度谱分布和大气能见度的影响

于2013年1月连续在线观测天津城区气溶胶数浓度谱分布和大气能见度,并结合相关气象资料,探讨相对湿度(RH)对气溶胶浓度谱分布和大气能见度的影响.结果表明,观测期间发生了4次连续雾霾天气过程,4次雾霾天气过程对应着气溶胶粒子数浓度的连续高值,低能见度天气系高浓度气溶胶粒子和高相对湿度协同所致;随着RH增大,PN1和PN2.5-10呈增长趋势,RH90%后,PN1和PN2.5-10有所降低,PN1-2.5则持续增长,高RH对气粒转化和气溶胶粒子的碰并聚合作用明显;气溶胶吸湿增长因子计算表明,高RH下水汽对能见度影响很大,尤其是大雾天气下其影响甚至可能超过气溶胶粒子浓度对其的影响.     

大气气溶胶粒径分布特征与呼吸系统暴露评估研究进展

近年来气溶胶污染被社会各界密切关注.大气气溶胶的粒径分布和污染物组成特征研究是探究大气气溶胶污染成因的基础,同时也是准确评估人体暴露于气溶胶污染导致的健康风险的关键.多级采样器可分粒径采集大气气溶胶,通过模拟人体呼吸系统进而准确量化大气气溶胶组分被吸入后在人体的沉积部位和沉积量,从而被应用至大气气溶胶粒径分布特征和人体健康风险评估的研究中.本文介绍了大气气溶胶粒径分级方法,探讨了应用多级采样器在气溶胶粒径分布研究中存在的主要问题及解决方案,并综述了大气气溶胶粒径分布特征和人体呼吸系统暴露评估的研究进展,最后结合当前的研究现状对大气气溶胶在粒径分级和人体健康风险研究领域的未来发展方向进行了展望.     

北京及周边地区大气近地面层真菌气溶胶的变化特征

2005年4月~2006年10月期间,利用Andersen六级空气生物采样器分别在北京、兴隆和香河3地区不同的季节进行外场采样观测,研究了大城市及其周边地区近地面层大气中真菌气溶胶菌群种类与浓度,粒度的季节变化规律及其分布特征.研究发现,3地区大气中真菌气溶胶的生物多样性变化明显,其优势菌群类型的季节变化显著;3地区大气真菌气溶胶数浓度的季节变化规律各不相同;北京市大气中真菌气溶胶数浓度的日变化显著,但未发现固定模式.     

东海大气气溶胶中二元羧酸的分布特征及来源

大气气溶胶中的二元羧酸因其在全球气候变化中的潜在作用而受到广泛关注.利用2011年5月12日-6月6日在东海采集的气溶胶样品,分析其中水溶性二元羧酸及常量离子浓度,探讨东海气溶胶中二元羧酸的时空分布特征及来源.结果显示东海大气气溶胶中乙二酸、丙二酸和丁二酸的浓度分别为26.0～1475.5 ng·m-3、0.1 ～61.4 ng·m-3和0.1～132.4 ng·m-3,乙二酸在这3种二元羧酸中的贡献最大,为88.3％.东海气溶胶中二元羧酸浓度的昼夜变化不显著.空间分布整体呈现近海高、远海低的趋势.气团的来源和迁移路径以及气象因素影响气溶胶中二元羧酸的分布,气团来自污染较重的陆源时气溶胶中二元羧酸的浓度较高,气团来自清洁的海洋源时,二元羧酸的浓度则较低;阴雾天气时气溶胶中二元羧酸浓度相对较高,降雨发生时二元羧酸的浓度较低.二元羧酸与常量离子的相关性分析表明,自然源和人为源释放的挥发性有机物质在液相中氧化生成二元羧酸是东海大气气溶胶中二元羧酸的主要源,而汽车尾气和生物质燃烧的一次排放、海洋源以及碱性粗颗粒吸收气体二元羧酸不是主要源.液相中乙醛酸氧化形成的乙二酸和长链二元羧酸氧化形成的乙二酸对东海气溶胶中乙二酸的贡献分别为41％和59％.     

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.     

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.