杭州大气颗粒物散射消光特性及霾天气污染特征

2011年7月~2012年6月期间,对大气散射系数、颗粒物浓度及气象因子进行同步观测,以评估颗粒物散射消光对杭州市大气能见度的影响.结果表明,杭州市大气颗粒物散射系数日均值变化范围为108.4~1 098.1 Mm-1,年均值为428.62Mm-1±200.2 Mm-1.散射系数呈明显的季节变化,秋冬高,夏季低.日变化呈典型的双峰型,早峰出现在08:00,晚峰出现在21:00.PM2.5和PM10的散射效率分别为7.6 m2·g-1和4.4 m2·g-1,颗粒物散射消光占总消光比例的90.2%.灰霾和重度灰霾天气下,散射系数分别为684.4 Mm-1±218.1 Mm-1和1 095.4 Mm-1±397.7 Mm-1,达到非霾天气的2.6和4.2倍,表明颗粒物散射消光作用是导致杭州市大气能见度下降和灰霾天气发生的主要因素.     

北京2013年1月连续强霾过程的污染特征及成因分析

以北京市2013年1月份连续灰霾天气中10~16日的强霾污染过程为例,利用MPL-4B型IDS系列微脉冲激光雷达观测资料由Fernald算法反演得到此次污染过程中气溶胶垂直分布特性,结合地面气象条件和天气形势分析污染原因,并讨论与气溶胶地面监测数据的符合性.结果表明:此次连续强霾过程污染严重,观测时段内89.4%的时间出现霾,39.8%的污染时段达到重度霾级别,其中大气地表消光系数与PM2.5浓度变化呈显著线性相关关系,相关系数达0.95.研究过程内,大气边界层在91%的时段低于500m,平均仅为293m,低边界层抑制了污染物的有效扩散;近地面垂向各高度的消光系数持续达到1.5km-1以上,对比气溶胶退偏比发现城市上空的大气强消光为气溶胶颗粒物和大气水分共同导致;气溶胶光学厚度(AOD,532nm)较大,有83.6%的时段超过1,且受相对湿度影响较大,相对湿度偏小时段的AOD值主要为气溶胶颗粒贡献,相对湿度较大时段,细颗粒物吸湿增长导致AOD受大气水分干扰显著.连续静稳的天气形势和区域污染是导致此次强霾发生和持续的主要原因,高湿天气则加剧了灰霾状况.     

南京地区一次灰霾天气的微脉冲激光雷达观测分析

利用微脉冲激光雷达(MPL)对2012年10月南京地区的一次灰霾天气进行了不间断观测,结合地面气象要素和PM10、PM2.5质量浓度资料分析了此次污染过程颗粒物质量浓度、气象要素、气溶胶垂直方向光学特性和混合层高度(MLH)日变化趋势以及相关性并与11月11~12日非灰霾天气做了消光系数和MLH的比较.结果表明,本次灰霾天气颗粒物浓度与近地面消光系数日变化较相似,基本上呈现夜间高午后低的趋势;灰霾期间MLH峰值滞后于地面温度峰值2h,MLH与PM2.5呈现负相关关系,两者相关系数为-0.57;霾天MLH远低于非灰霾天;霾期间近地面消光系数大部分时刻大于1.0km-1,远大于非霾日0.1~0.25km-1范围的消光系数.     

基于微脉冲激光雷达的上海浦东地区不同强度霾研究

利用微脉冲激光雷达(MPL)对上海浦东2008年12月1日至2010年11月31日期间连续观测的霾期间气溶胶的消光特性进行分析,讨论了上海浦东地区不同强度霾和无霾时气溶胶的垂直分布日变化与季节变化.结果表明,重、中度霾的气溶胶主要分布在500m以下,小时平均消光系数值在0~1.2km-1范围内波动;轻度霾及轻微霾时段,小时平均消光系数波动范围约在0~0.5km-1;无霾时段小时平均消光系数波动范围约在0~0.2km-1;中-重度霾时段消光系数春>冬>夏>秋;夏季低层大气消光较大,春季高层大气消光较大,冬秋两季随高度增加消光逐渐减小;夏冬两季较易发生中、重度霾.     

天津城区春季大气气溶胶消光特性研究

利用天津大气边界层观测站2011年4月1日~5月10日气溶胶散射系数、吸收系数、PM2.5质量浓度、大气能见度和常规气象观测数据,分析了气溶胶散射系数和吸收系数的变化特征,以及气溶胶消光系数与PM2.5质量浓度和大气能见度的关系,并对两种方法计算的消光系数进行了比较.结果表明,观测期间天津城区气溶胶散射系数为369.93 Mm-1,对大气消光贡献为86.7%,气溶胶吸收系数为36.32 Mm-1,对大气消光贡献为8.5%,单次散射反照率为0.91;气溶胶散射系数和吸收系数的日变化特征具有明显的双峰结构,对应于早晚交通高峰;不同天气类型下其日分布特征存在较大差异,霾日散射系数和吸收系数最高,沙尘日和降水日次之,晴日最低;气溶胶散射系数和吸收系数与PM2.5质量浓度呈线性正相关,与大气能见度呈指数负相关,观测期间气溶胶质量散射效率均值为2.95m2/g;采用Koschmieder’s公式反算能见度获得的大气消光系数,与通过测量气溶胶散射系数、气溶胶吸收系数、气体散射系数和气体吸收系数等分量加和获得的消光系数相比一致性较好,高相对湿度天气下能见度反算值高于各系数加和值.     

上海秋季典型大气高污染过程中有机碳和元素碳的变化特征

于2011年10月1日至10日在上海市城区对大气中细粒子的质量浓度和含碳气溶胶进行了在线连续观测,获得了秋季典型大气灰霾污染过程中含碳气溶胶的变化特征.观测结果显示,在大气灰霾过程中PM2.5中有机碳(OC)和元素碳(EC)的质量浓度分别为(20.38±7.11)μg·m-3和(4.07±1.97)μg·m-3,浓度显著高于非霾过程.以非霾天气的起始点作为参照点,得出灰霾期间OC和EC的增长率分别为641％±258％和409％±246％,本次灰霾过程中OC的污染累积与二次生成作用分别占63.8％和36.2％,污染过程以累积为主.灰霾期间OC/EC与O3具有良好的线性关系,且相关分析表明二者之间呈正相关,OC浓度的升高与含碳组分的光化学反应有关.采用EC示踪法估算短期大气过程中有机碳(SOC)含量,灰霾天气和非霾天气PM2.5中的SOC浓度分别为1.64～17.96 μg·m 3和0.25 ～2.83 μg·m-3,分别占OC的l0.7％～66.7％和9.2％ ～52.5％.     

基于自动站资料的苏州灰霾天气分析

利用苏州2010~2013年的逐时气象和大气成分观测资料,对苏州灰霾天气特征进行了统计分析,研究发现:苏州灰霾的小时频率为30.7%,灰霾等级以轻微灰霾为主,干霾占总灰霾的比例为85.6%.2013年12月灰霾小时频率最高,达82.3%.灰霾小时频率有明显的日变化特征,峰值出现在上午8:00时,达36.3%,14:00~16:00时,灰霾频率最低,约为25%左右;灰霾期间,PM10、PM2.5、PM1.0和散射系数分别是非灰霾期间的1.72、2.07、1.88和2.58倍.采用不同的灰霾日标准,苏州年均灰霾日数在94~243之间,相差极大.灰霾频率和气象条件有密切关系,灰霾频率最高的相对湿度区间为70%~80%,重度霾最多出现在90%~95%的相对湿度条件下;随风速增加,灰霾频率逐渐下降,在西北风向下,灰霾频率最大.大气消光以颗粒物散射消光为主,约占总消光的82%左右,黑碳的吸收消光约占13%左右.     

杭州黑碳气溶胶污染特性及来源研究

2011年7月~2012年6月对黑碳气溶胶(BC)、PM2.5、污染气体及气象因子进行同步观测,以评估杭州市BC污染特征、来源分布及对大气能见度的影响.结果表明:杭州市大气BC日均浓度范围为1.3~16.5μg/m3,年均值达到(5.1±2.5)μg/m3.BC呈明显的季节变化趋势,秋冬季高,夏季低.BC也呈典型的日变化趋势,交通高峰期高,下午低,同时与NOx呈较好的相关性,表明城市中BC受到机动车尾气排放的重要影响;而BC/CO低于其他城市则表明生物质燃烧排放可能是杭州BC的另一大重要来源.BC随风速下降呈上升趋势, BC超过10μg/m3的高浓度事件中,风速基本低于2m/s,北-西北-西风对高浓度BC的输送作用明显.观测期间BC的吸收系数为(44.8±23.0)Mm-1,占到总消光比例的10.4%.灰霾和重度灰霾天气下,吸收系数分别为(66.2±30.1),(100.2±49.2)Mm-1,达到非霾天气的2.2和3.4倍, 表明BC吸收消光作用是影响杭州市大气能见度下降和灰霾天气发生的重要因素之一.     

济南秋季霾与非霾天气下气溶胶光学性质的观测

应用黑碳仪和积分浊度计于2009年10月11日至11月18日针对济南市大气气溶胶的光学特性进行了观测.结果显示,观测期间霾天气的散射系数和吸收系数及非霾天气的散射系数和吸收系数平均值分别为(582.5±311)Mm-1、(680.2±47.2)Mm-1和(205.7±134.8)Mm-1、(31.0±25.8)Mm-1.霾天气的气溶胶散射系数和吸收系数分别为非霾天气的2.6倍和2.8倍,单词散射反照率(SSA)也高于非霾天气.霾天气中二次气溶胶生成及黑碳气溶胶聚集是改变吸收系数、散射系数和SSA的日变化趋势的重要原因.此外,估算了观测期间及霾和非霾天气中气溶胶的光学厚度(AOD)分别为0.78,1.14和0.47.后向气流轨迹分析显示,非霾天气的气流主要来自于济南的西北至东北方向,运动速度快;而霾天气的所有的气流均来自于济南西南至东南方向,运动速度慢,当气流经过山东南部的火点时加剧了济南市的霾,并严重影响到该地区大气气溶胶的光学性质.     

一次严重灰霾过程的气溶胶光学特性垂直分布

利用激光雷达在广州地区一次严重灰霾过程进行探测,并反演气溶胶消光系数及退偏比,分析边界层结构演变对气溶胶消光系数廓线分布的影响.结果表明,气溶胶主要在1.5km以下.发生灰霾天气时,霾层达到1km,午后可达1.5km,发生严重灰霾天气时,霾层只有500m.气溶胶消光系数随高度分布在清洁过程中呈线性递减,标高为1490m,在灰霾过程中呈指数递减,标高为789.5m.从气溶胶消光系数廓线变化可以很好地反演边界层结构的演变.气溶胶消光系数在残留层顶出现极大值.气溶胶退偏比有明显的日变化,白天的退偏比比夜间的高,午后出现峰值.该次过程气溶胶的退偏比小于0.2.本地气溶胶廓线只有在清洁过程时与Elterman廓线接近.     

Evaluation of phytoextracting cadmium and lead by sunflower, ricinus, alfalfa and mustard in hydroponic culture

Soil contaminated with heavy metals cadmium(Cd)and lead(Pb)is hard to be remediated.Phytoremediation may be a feasible method to remove toxic metals from soil,but there are few suitable plants which can hyperaccumulate metals.In this study,Cd and Pb accumulation by four plants including sunflower(Helianthus annuus L.),mustard(Brassica juncea L.),alfalfa(Medicago sativa L.), ricinus(Ricinus communis L.)in hydroponic cultures was compared.Results showed that these plants could phytocxtract heavy metals, the ability of accumulation differed with species,concentrations and categories of heavy metals.Values of BCF(bioconcentration factor)and TF(translocation factor)indicated that four species had dissimilar abilities of phytoextraction and transportation of heavy metals.Changes on the biomass of plants,pH and Eh at different treatments revealed that these four plants had distinct responses to Cd and Pb in cultures.Measurements should be taken to improve the phytoremediation of sites contaminated with heavy metals,such as pH and Eh regulations,and so forth.     

Oxidation of As(Ⅲ) by potassium permanganate

The oxidation of As(Ⅲ) with potassium permanganate was studied under conditions including pH, initial As(Ⅲ) concentration and dosage of Mn(Ⅶ). The results have shown that potassium permanganate was an effective agent for oxidizing of As(Ⅲ) in a wide pH range. The pH value of tested water was not a significant factor affecting the oxidation of As(Ⅲ) by Mn(Ⅶ). Although theoretical redox analyses suggest that Mn(Ⅶ) should have better performance in oxidization of As(Ⅲ) within lower pH ranges, the experimental results show that the oxidation efficiencies of As(Ⅲ) under basic and acidic conditions were similar, which may be due to the adsorption of As(Ⅲ) on the Mn(OH)2 and MnO2 resulting from the oxidation of As(Ⅲ).     

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.     

Chlorobenzenes in waterweeds from the Xijiang River （Guangdong section） of the Pearl River

The Xijiang River is the major source of water for about 4.5 millions of urban population and 28.7 millions of rural population. The water quality is very important for the health of the rural population. The concentration and distribution of chlorobenzenes (CBs) in both water and waterweeds collected from 4 stations in the Xijiang River (Gangdong section) of the Pearl River in April and November were determined. The result showed that nearly every congener of CBs was detected. The total contents of CBs (∑CBs) in the river water ranged from 111.1 to 360.0 ng/L in April and from 151.9 to 481.7 ng/L in November, respectively. The pollution level of CBs in the water in April was higher than that in November. The contents of ∑ CBs in waterweeds ranged from 13.53×102 μg/g to 38.27×102μg/g dry weight (dw). There was no significant difference between April and November in waterweeds. The distribution of CBs in roots, caulis, and leaves of Vallisneria spiralis L. showed different patterns. The leaves mainly contained low-molecular-weight CBs(DCBs), whereas the roots accumulated more PCBs and HCBs. The average lgBCFlip (bioconcentration factor) of CBs ranged from 0.64 to 3.57 in the waterweeds. The spatial distribution character of CBs in the Xijiang River was: Fengkai County ＜ Yunan County ＜Yun'an County ＜ Gaoyao County according to the ∑CBs, and the pollution deteriorated from the upstream to the downstream of the Xijiang River. Further analysis demonstrated that the discharge of waste containing CBs may be the main source of CBs pollution in the Xijiang River.     

Degradation of 2,4-dichlorophenol with a novel TiO2/Ti-Fe-graphite felt photoelectrocatalytic oxidation process

Degradation of 2,4-dichlorophenol(2,4-DCP)was studied in a novel three-electrode photoelectrocatalytic(PEC)integrative oxidation process,and the factors influencing the degradation rate,such as applied current,flow speed of O_2,pH,adscititious voltage and initial 2,4-DCP concentration were investigated and optimized.H_2O_2 was produced nearby cathode and Fe~(2 )continuously generated from Fe anode in solution when current and O_2 were applied,so,main reactions,H_2O_2-assisted TiO_2 PEC oxidation and E-Fenton reaction,occurred during degradation of 2,4-DCP in this integrative system.The degradation ratio of 2,4-DCP was 93% in this integrative oxidation process,while it was only 31% in E-Fenton process and 46% in H_2O_2-assisted TiO_2 PEC process.So,it revealed that the degradation of 2,4-DCP was improved greatly by photoelectrical cooperation effect.By the investigation of pH,it showed that this integrative process could work well in a wide pH range from pH 3 to pH 9.     

Effect of copper on the degradation of pesticides cypermethrin and cyhalothrin

The influence of coexisting copper (Cu) ion on the degradation of pesticides pyrethroid cypermethrin and cyhalothrin in soil and photodegradation in water system were studied.Serial concentrations of the pesticides with the addition of copper ion were spiked in the soil and incubated for a regular period of time,the analysis of the extracts from the soil was carried out using gas chromatography (GC).The photodegradation of pyrethroids in water system was conducted under UV irradiation.The effect of Cu~(2 ) on the pesticides degradation was measured with half life (t_(0.5)) of degradation.It was found that a negative correlation between the degradation of the pyrethroid pesticides in soil and Cu addition was observed.But Cu~(2 ) could accelerate photodegradation of the pyrethroids in water.The t_(0.5) for cyhalothrin extended from 6.7 to 6.8 d while for cypermethrin extended from 8.1 to 10.9 d with the presence of copper ion in soil.As for photodegradation,t_(0.5) for cyhalothrin reduced from 173.3 to 115.5 rain and for cypermethrin from 115.5 to 99.0 min.The results suggested that copper influenced the degradation of the pesticides in soil by affecting the activity of microorganisms.However, it had catalyst tendency for photodegradation in water system.The difference for the degradation efficiency of pyrethroid isomers in soil was also observed.Copper could obviously accelerate the degradation of some special isomers.     

基于综合水质标识指数和对应分析法的校园河道水质评价

以三峡大学的校园河道求索溪为研究对象,利用综合水质标识指数法确定求索溪水质类别,分析其水质时空变化规律,并利用对应分析法得出求索溪中不同监测点的主要污染因子.研究结果表明:求索溪整体的综合水质标识指数为7.423,整体水质为劣V类(地表水环境质量标准GB 3838-2002)且黑臭.从时间变化来看,求索溪4月份的水质最差,5月份次之,4、5月份所有监测点的水质都劣于V类且黑臭;8月份水质最好,水质为Ⅳ类;从空间分布来看,8个监测点综合水质标识指数均超过6.0,水质为劣V类,其中6号监测点的水质相对最好,监测点3号的水质相对最差;对应分析法得出求索溪的整体水体污染程度受总氮因子的影响最大,其次为总磷.该研究拟为求索溪及类似校园河道的水环境治理研究提供基础依据和参考.