天津污染天气边界层温度层结变化特征及预报阈值确定

针对天津市大气污染防治需求,基于2016年4月1日—2017年3月31日天津255 m气象塔观测资料及数值模拟,开展天津地区污染天气边界层温度层结变化特征及预报阈值研究.结果表明:(1)天津地区10~250 m高度的气温递减率为0.56℃/100 m,当日均气温递减率小于0.4℃/100 m时,垂直扩散条件不利于大气污染物扩散,出现中度以上污染概率为64%,重污染概率为47%.从温度廓线和逆温频率统计分析,贴地逆温占所有逆温的55%,除贴地逆温以外逆温底部最易出现在160 m的高度,大量脱地逆温的出现不利于高架源夜间的排放.(2)每年10月—次年2月天津逆温频率为20%,冬季需要关注逆温情况对大气污染物扩散的影响.如秋、冬季8:00逆温仍然存在,重污染天气出现概率高达56%,中度及以上污染出现概率为72%,是重污染天气辨识的重要指标.(3)7:00—10:00在逆温消散或者日均气温递减率由0.6℃/100 m向0.4℃/100 m变化时,任何细微变化对大气垂直扩散有显著影响.基于天津地区PM_(2.5)污染情况下,数值模拟显示10~250 m的气温递减率由于气溶胶的存在可减少0.06℃/100 m,在25个重污染过程中,日均气温递减率平均下降0.18℃/100 m,对大气垂直扩散条件产生显著影响.因此,在空气污染预报分析时使用不考虑气溶胶辐射效应的天气模式分析温度层结,需要适当调整阈值,尤其是在7:00—10:00逆温消散及垂直温度递减率由0.6℃/100 m向0.4℃/100 m变化时.     

21世纪以来天津细颗粒物气象扩散能力趋势分析

基于高精度的排放源和大气化学模式WRF/chem,在同排放源条件下模拟了2000~2015年天津地区PM_(2.5)质量浓度,根据NECP再分析资料和地面观测相关数据构建细颗粒物气象扩散指数,使用两种方法描述21世纪以来天津地区细颗粒物气象扩散能力变化趋势.研究结果表明:2000~2015年期间天津地区细颗粒气象扩散能力呈现周期性波动,不利气象条件的第一个峰值出现在2003~2004年,第二个峰值为2013~2015年,两个峰值相距11年,在2000~2015年间,天津地区气象扩散能力(主要针对PM_(2.5)影响)年际平均波动4.1%,最大值约为9%,对于大气污染防治目标制定和效果评估,必须考虑气象年际波动的影响;2008~2010年气象条件较有利于细颗粒物扩散,此后逐年转差,在2013~2015年处于历史正距平(不利扩散),从而导致2013~2015年雾霾和重污染天气频发;2015年相比2013年天津细颗粒物气象扩散能力没有明显提高,但PM_(2.5)质量浓度下降29%,大气污染防治措施的有效执行在其中发挥积极作用.     

上海典型持续性PM2.5重度污染的数值模拟

本研究针对2013年1月23~24日的上海PM_(2.5)持续重污染过程,采用WRF-Chem大气化学模式以及PM_(2.5)质量浓度、能见度、气象要素等地面实测资料相结合的方式,揭示了造成上海冬季PM_(2.5)持续性重污染的一类"天气学必要成因",即一次弱冷空气活动过程导致了两种不利污染天气条件——"弱气压场(静稳形势)"和"弱冷空气扩散(输送形势)",两者先后影响上海造成PM_(2.5)浓度持续上升.主要过程如下:首先弱冷空气影响之前,上海处在不利的局地气象扩散条件下,受弱气压场控制10 h后本地PM_(2.5)质量浓度达到重度污染水平,之后夜间稳定边界层(地面静风和低层逆温)使得PM_(2.5)重度污染维持了7h,期间PM_(2.5)平均质量浓度为172.4μg·m~(-3).后期弱冷空气影响上海,虽然改善了局地扩散条件但是同时产生了明显的周边污染物输送,使得本地PM_(2.5)质量浓度升高并达到峰值(280μg·m~(-3)),继续加重污染水平,期间PM_(2.5)平均质量浓度为213.6μg·m~(-3).WRF-Chem模拟结果进一步表明,整个污染过程周边区域输送对上海PM_(2.5)平均贡献率为23%,其中两个阶段周边区域输送的平均贡献率分别为17.2%和32.2%,可见在不同的污染天气条件下周边污染源的贡献存在显著差异,因此可以根据对污染天气类型的预判制定应急减排方案.     

昆明低空大气温度层结特征与空气质量的Logistic判别模型

低空大气逆温及地面风速是影响空气质量变化的主要气象条件,特别是逆温的频率、强度制约着大气污染物聚积和扩散。定义了1km以下低空大气的温度层结强度。利用昆明L波段探空雷达加密数据,统计了2014—2018年08 h探空数据温度层结特征,分析了逆温的频率、强度和地面风速等气象要素与空气质量的相关性,建立基于Logistic判别方法的昆明空气质量指数和PM_(2.5)浓度的拟合模型。结果显示:基于定义的温度层结强度的统计,昆明1km以下低空大气整层的逆温发生频率10.7%,年平均强度0.13℃·(100m)~(-1),逆温的频率和强度月变化曲线与轻度污染及PM_(2.5)浓度的变化联系密切;温度层结强度和地面风速通过了α=0.05的相关系数显著性检验,与空气质量指数和PM_(2.5)浓度相关性好,最佳的气象要素因子的相关系数可达到0.3660;Logistic判别模型对轻度污染的拟合准确率在66.3%以上,优良空气的拟合准确率在72.5%以上;对PM_(2.5)浓度超标的拟合准确率在59.9%以上,PM_(2.5)一级浓度的拟合准确率在68.8%以上。     

邯郸一次重污染天气过程分析

利用常规气象观测资料和邯郸环境监测资料,针对邯郸2015年12月26日下午PM_(10)和PM_(2.5)污染指数骤升的重污染天气过程,从逐时污染指数变化、气象要素的演变、气象扩散条件和逐时地面要素场特征等方面进行了分析。结果表明:PM_(10)和PM_(2.5)污染指数的陡升与气温骤降、相对湿度骤升相对应;逆温层的存在不利于空气污染物的扩散;地面风场的辐合早于污染指数的快速增加,地面风速逐渐增大和北方湿冷空气的南下,与污染指数陡升相对应,导致本次重污染天气过程的产生。     

基于无人机探空和数值模拟天津一次重污染过程分析

污染发生在边界层中,边界层热力和动力垂直结构对重污染天气形成有显著影响.本文基于无人机探空、地基遥感观测和数值模式,开展天津地区2019年1月10~15日重污染过程期间边界层垂直结构及污染成因分析,以期加强北方沿海城市边界层过程对重污染影响规律认知,提升重污染天气预报预警准确率.结果表明：大气温度层结对重污染天气形成、持续和消散有显著影响,此次过程伴随逆温层的发展和消散,PM_2.5高浓度区白天向大气上层发展,高度可达300 m以上,夜间向近地面压缩,高度在100 m左右;雾天气出现并在白天维持,改变了边界层垂直结构特征,雾顶逆温的持续存在抑制了污染物向大气上层扩散,使得白天湍流垂直混合过程贡献明显下降,导致近地面重污染天气维持和发展;过程期间区域输送贡献率为66.6%,边界层垂直结构与重污染天气区域输送密切相关,区域污染物输送高度主要出现在边界层顶部以及雾顶逆温层以上的大风速层处,且随着边界层和雾顶抬升高度的变化,通过下沉运动影响地面,形成北部弱高压天气控制下静稳天气区域输送;边界层垂直结构影响冷空气对空气质量的改善效果,S3阶段雾顶的强逆温导致冷空气无法通过湍流切应力传导到地面,在高低空存在明显的风速差,冷空气影响地面时间延后,作用减弱,重污染天气无法彻底缓解.     

基于天气背景天津地区重污染天气特征分析

以天津地区长序列观测PM_(2.5)质量浓度资料为依托,基于天气背景对2014—2016年天津地区重污染天气特征进行分析,并以此为基础评估天津环境气象数值模式(WRF/Chem)在不同天气条件下的模拟效果.结果显示:2009—2016年天津地区重污染天气为341 d,约占全部天数的11.7%,重污染天气主要出现在每年的10月—次年3月,约占全年的82%,重污染天气出现的地面形势主要为锋前低压区、低压槽前、均压场和高压后,4类天气类型占所有重污染天气的73%.同一天气背景下,PM_(2.5)质量浓度模拟值与实况值之间的误差有相似之处,低压槽天气时细颗粒污染浓度模拟明显偏低;冷锋前低压区、华北地形槽和低压过程模拟值略有偏低;高压前和高压底天气模拟值略微偏高;数值模式天津地区重污染TS(Threat score)评分为0.68,漏报与低压槽辐合线模拟位置偏差、冷空气受污染反馈作用影响、小尺度闭合低压区未准确模拟3个因素密切相关;空报主要与冷空气过程影响时间模拟偏差、高压中心位置偏差及其输送通道建立时间影响密切相关.     

城市森林植被区空气PM_(2.5)质量浓度时空变化

该研究选取北京大兴南海子公园植被区与亦庄非植被区PM_(2.5)数据进行研究,对比分析植被区与非植被区PM_(2.5)质量浓度日变化、月变化和年变化特征,典型天气下的PM_(2.5)质量浓度变化。结果表明:植被区PM_(2.5)质量浓度整体上低于非植被区,二者日变化均呈典型的双峰曲线,白天低,夜间高,最小值出现在下午15:00左右;从不同月份看,PM_(2.5)质量浓度最高值出现在冬季的1月、2月,最低值出现在6月、8月,整体表现为冬季月份明显高于其余月份;气温、降雨和大风均与PM_(2.5)浓度呈负相关,晴天时,温度较高,有利于PM_(2.5)浓度降低;降雨有利于空气颗粒物沉降,有效清除大气PM_(2.5)污染,降低其浓度;大风天气会增加大气环流,有助于颗粒物在大气中扩散,使PM_(2.5)不易滞留,从而导致浓度降低。降雨和大风均能导致PM_(2.5)污染降低,且城市森林植被对于PM_(2.5)有明显降低作用。     

成都市污染边界层高度的演变特征分析

基于2014年1月21日至2月5日成都市人民南路四段逐时PM_(2.5)质量浓度、大气能见度资料以及同期Mie散射激光雷达探测数据,遵循消光系数与细颗粒物质量浓度之间的关系,探讨污染边界层高度的演变特征。结果表明:污染时段内的污染边界层高度偏低,平均为221m;污染边界层高度与地面PM_(2.5)浓度的变化具有明显相关性,但污染边界层高度改变在前,地面PM_(2.5)浓度响应在后;污染边界层高度的日变化表现为单峰单谷型,峰值和谷值分别出现在08:00时和14:00时前后。     

2015年“十一”期间北京市大气重污染过程分析

采用垂直观测、地面观测、PM_(2.5)化学组分观测和气团轨迹分析等手段,对2015年10月份北京市一次大气重污染过程进行了分析.结果表明,重污染时近地面层气溶胶消光系数升高,污染物主要积聚在600m以下.重污染期间气象要素特征为:风场弱,湿度大,地面受弱气压场控制,边界层高度极低.重污染期间不同站点PM_(2.5)浓度变化趋势和峰值出现时间较为一致;大部分时段PM_(2.5)中NO_3~-浓度明显高于其他组分;周边区域受重污染的影响面积相对较小,高浓度区主要集中在北京市及近周边地区.多手段的观测结果以及PM_(2.5)浓度与气象要素和各化学组分的相关性分析的结果均表明:区域传输,包括秸秆焚烧,对本次北京市重污染天气过程具有一定的影响,但本地机动车排放在不利气象条件下的积累、二次转化以及垂直方向空间的极端压缩是导致重污染的主要原因.     

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.     

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.     

Effects of chitosan on growth of an aquatic plant (Hydrilla verticillata) in polluted waters with different chemical oxygen demands

Effects of chitosan on a submersed plant, Hydrilla verticillata, were investigated. Results indicated that H. venicillata could prevent ultrastructure phytotoxicities and oxidativereaction from polluted water with high chemical oxygen demand (COD). Superoxide dismutase (SOD) activity and malondialdehyde (MDA) contents in H. verticillata treated with 0.1% chitosan in wastewater increased with high COD (980 mg/L) and decreased with low COD (63 mg/L), respectively. Ultrastructural analysis showed that the stroma and grana of chloroplast basically remained normal. However, plant cells from the control experiment (untreated with chitosan) were vacuolated and the cell interval increased. The relict of protoplast moved to the center, with cells tending to disjoint. Our findings indicate that wastewater with high COD concentration can cause a substantial damage to submersed plant, nevertheless, chitosan probably could alleviate the membrane lipid peroxidization and ultrastructure phytotoxicities, and protect plant cells from stress of high COD concentration polluted water.     

Removal of cadmium using MnO2 loaded D301 resin

MnO2 loaded weak basic anion exchange resin D301 （Anion exchange resin, macroreticular weak basic styrene） as adsorbent has been prepared and applied to the removal of cadmium. The adsorption characteristics have been investigated with respect to effect of pH, equilibrium isotherms, removal kinetic data, and interference of the coexisting ions. The results indicated that the Cd^2＋ could be efficiently removed using MnO2 loaded D301 resin in the pH range of 3-8 from aqueous solutions with the co-existence of high concentration of alkali and alkaline-earth metals ions. The saturate adsorption capacity of the Cd^2＋ was 77.88 mg/g. The adsorption process followed the pseudo first-order kinetics. The equilibrium data obtained in this study accorded excellently with the Langmuir adsorption isotherm.     

Effect of coagulation pretreatment on the fouling of ultrafiltration membrane

The purpose of this study is to understand the effect and mechanism of preventing membrane fouling, by coagulation pretreatment, in terms of fractional component and molecular weight of natural organic matter （NOM）. A relatively higher molecular weight （MW） of hydrophobic compounds was responsible for a rapid decline in the ultrafiltration flux. Coagulation could effectively remove the hydrophobic organics, resulting in the increase of flux. It was found that a lower MW of neutral hydrophilic compounds, which could remove inadequately by coagulation, was responsible for the slow declining flux. The fluxes in the filtration of coagulated water and supernatant water were compared and the results showed that a lower MW of neutral hydrophilic compounds remained in the supernatant water after coagulation could be rejected by a membrane, resulting in fouling. It was also found that the coagulated flocs could absorb neutral hydrophilic compounds effectively. Therefore, with the coagulated flocs formed on the membrane surface, the flux decline could be improved.     

Penetration analysis of elements and bioleaching treatment of spent refractory for recycling

Acidithiobacillus ferrooxidans ATCC23270 and Acidithiobacillus thiooxidans TM-32 were used for bioleaching of spent refractories of aluminium and copper melting furnaces for their recycling.Firstly,penetration of elements into aluminium melting furnace refractory was investigated and it was found that up to 7 cm from surface was contaminated.Comparison on leaching efficiency by the strains ATCC23270 and TM-32 found that the strain ATCC23270 could treat larger amount of the refractories than the strain TM-32 could do.In the experiment of bioleaching of spent refractory aluminium melting furnace by the strain ATCC23270,high leaching efficiency were obtained on Al,Si,and Ca,and extremely low leaching performance was,however,shown on the rest of elements i.e.,Na,Mn,and Zn.Under the strain TM-32 use,relatively high leaching performance was recognized on Al,Si,Ca,Na,Mn,and Zn.In the experiment of bioleaching for spent refractory copper melting furnace,almost the same leaching trends were shown on Cu,Zn,Al,and Si under the strains ACTT23270 and TM-32 uses.     

Simultaneous removal of ammonium and phosphate by zeolite synthesized from coal fly ash as influenced by acid treatment

Zeolite synthesized from fly ash （ZFA） without modification is not efficient for the purification of NH4＋ and phosphate at low concentrations that occur in real effluents, despite the high potential removal capacity. To develop an effective technique to enhance the removal efficiency of ammonium and phosphate at low concentrations, ZFA was modified with acid treatment and the simultaneous removal of ammonium and phosphate in a wide range of concentration was investigated. It was seen that when compared with untreated ZFA, only the treatment by 0.01 mol/L of H2SO4 significantly improved the removal efficiency of ammonium at low initial concentrations. The behavior was well explained by the pH effect. Treatment by more concentrated H2SO4 led to the deterioration of the ZFA structure and a decrease in the cation exchange capacity. Treatment by 0.01 mol/L H2SO4 improved the removal efficiency of phosphate by ZFA at all initial P concentrations, while the treatment by concentrated H2SO4 （≥0.9 mol/L） resulted in a limited maximum phosphate immobilization capacity （PIC）. It was concluded that through a previous mild acid treatment （e.g. 0.01 mol/L of H2SO4）, ZFA can be used in the simultaneous removal of NH4＋ and P at low concentrations simulating real effluent.