汾渭平原复杂地形影响下冬季PM2.5污染分布特征、来源及成因分析

汾渭平原受其复杂地形特征及产业结构影响,和京津冀、长三角地区一起被列为大气污染重点防治区域.本研究应用2014—2019年冬季中国环境监测总站汾渭平原各城市的六大空气污染物逐小时数据,结合欧洲中心ERA-5数据,利用HYSPLIT后向轨迹模型及T-model斜交旋转主成分分析法（PCT）,揭示过去6年汾渭平原冬季颗粒物浓度演变规律,厘清汾渭平原复杂地形影响下大气污染来源特征、潜在源区及成因,识别影响汾渭平原冬季空气污染的主要天气系统类型.HYSPLIT模拟结果表明,冬季喇叭口地形城市主要受本地和邻近区域污染源影响;山区盆地地形城市更易受到100~300 km距离以内污染源的传输影响,其中,来自陕北的气团对其影响最大;峡谷地形城市更易受到300~600 km范围内污染源的传输影响;平原地形城市的污染物浓度受区域传输的影响较大.影响汾渭平原冬季颗粒物重污染的天气系统可分为高压前部型、高压后部型、均压场型及低压倒槽型,其中,高压前部型是汾渭平原冬季重污染时段最易出现的天气形势.     

2017年汾渭平原东部大气颗粒物污染特征分析

高度集中的煤炭产业和繁忙的交通运输使得汾渭平原成为全国污染最严重的地区之一.利用中国环境监测总站发布的大气环境监测资料,以统计的方法分析了2017年汾渭平原东部三门峡市、运城市、渭南市、洛阳市的颗粒物质量浓度演变特征,并与北京市开展对比分析.结果表明:①2017年汾渭平原东部颗粒物污染形势较为严峻,ρ（PM_2.5）年均值范围为61~75 μg/m3,高于北京市（58 μg/m3）,ρ（PM_2.5）/ρ（PM₁₀）范围为0.47~0.57,远低于北京市的0.66,说明汾渭平原东部一次颗粒物的贡献更为显著.②与北京市相比,汾渭平原东部重污染有效时数较长,在三门峡市、运城市、渭南市和洛阳市出现PM_2.5重度及以上污染过程的时数分别占全年总时数的6.56%、8.91%、9.23%和9.10%.但由于汾渭平原东部重污染期间颗粒物质量浓度较北京市低,因此造成汾渭平原东部和北京市重度及以上污染过程中颗粒物质量浓度平均值在颗粒物质量浓度年均值中占比基本相同.③汾渭平原东部颗粒物质量浓度的周变化特征与北京市有显著区别.④重污染期间,汾渭平原东部ρ（PM_2.5）和ρ（PM₁₀）的日变化特征与ρ（SO₂）相同,均呈白天高、夜间低的特征,而北京市ρ（PM_2.5）和ρ（PM₁₀）的日变化特征与ρ（SO₂）相反,呈白天低、夜间高的特征,说明汾渭平原东部特殊的能源结构、边界层动力演变和局地环流造成高架点源对重污染期间污染物质量浓度的影响较显著.研究显示,汾渭平原东部应该加强重污染期间高架点源的管控.      

基于积累速率的汾渭平原秋冬季PM2.5污染特征及影响因素分析

为研究汾渭平原各城市PM_2.5污染特征及影响因素,利用2015—2019年汾渭平原11市秋冬季污染物逐时浓度,基于日变化分析构建了各城市慢速积累和快速积累的评价指标,量化了各城市的积累水平.结果表明：汾渭平原各城市PM_2.5积累水平差异显著,积累速率最快的城市是宝鸡,最慢的是三门峡;快速积累阈值最高的是临汾,最低的是三门峡.结合各地积累速率值的分布特征,11地市的积累水平可分为较强（宝鸡、临汾、吕梁、晋中）、中等（咸阳、渭南、铜川、运城、洛阳）和较弱（西安、三门峡）3种.积累速率多随浓度的增高呈上升趋势,其中吕梁和临汾最为显著,而西安增幅最小.从年变化来看,各地快速积累占比从2017年或2018年开始减少,从月变化来看,12月和1月为快速积累出现最多的月份.二次污染物和区域传输对PM_2.5积累速率均有影响,发生快速积累时,前体物SO₂和NO₂的浓度明显升高,二次反应显著;对临汾和西安的后向轨迹分析表明,西偏南方向气流的增加更易引起当地PM_2.5的快速积累.     

粤港澳大湾区吸收性气溶胶的解析

为了解粤港澳（Guangdong-Hong Kong-Macao,GHM）大湾区气溶胶污染现状,基于OMAERUV日产品数据,对粤港澳大湾区2008~2019年吸收性气溶胶指数（ultraviolet aerosol index,UVAI）的时空分布、未来趋势变化和潜在源区进行了分析,并对其影响因素进行了探讨.结果表明,GHM大湾区年时间序列上UVAI呈现出下降的趋势,年均下降为2.3%;月时间序列上从春季开始呈现倒"V"形,季节特征春季最高,冬、秋次之,夏季最低;空间上呈现中部区域一直属于高值区,12年年均UVAI高达0.35;UVAI分布在时间序列主要表现为可持续,有82.69%的区域在未来UVAI将呈现下降的趋势;GHM大湾区外部潜在源主要是东部工业产生的碳质源和海洋带来的生物源;UVAI潜在源区春季以碳质源和生物质源为主,夏季以生物质气溶胶源为主,秋季以碳质源占比最大,冬季沙尘性质气溶胶源有所增加;通过相关性分析,气溶胶和PM_2.5之间是相互依附的关系,工业生产活动是大气气溶胶的重要组成部分,降水可以降低大气中因工业生成所产生的气溶胶含量,第二产业活动在气温升高的情况下会加快气溶胶的生成.     

粘土矿物比率对沙尘源区的指示

为了探讨中国北方沙尘源区矿物组成特征并建立沙尘气溶胶的矿物示踪指标,在亚太地区气溶胶特征实验(ACE-Asia)期间对新疆阿克苏、甘肃敦煌、陕西榆林和内蒙古通辽沙尘气溶胶的矿物组成进行了研究.结果显示,中国主要沙尘源区沙尘气溶胶中高岭石与绿泥石的比率存在明显差异,西部沙尘源区(以阿克苏站点为代表)高岭石与绿泥石的比值较小(平均值为0.3),而北部沙尘源区(以榆林站点为代表)高岭石与绿泥石的比值相对较高(平均值为0.7).沉降区长武尘暴样品的粘土矿物比率和气团轨迹分析证实,在区域范围,高岭石与绿泥石的比值为较好的沙尘源区矿物示踪指标.而亚洲沙尘与撒哈拉沙尘的对比显示,高岭石与绿泥石的比值在全球范围有着沙尘源区指示的意义.     

汾渭平原临汾市2019年春节期间大气污染特征与来源解析

近年来汾渭平原冬季雾-霾事件频发,节假日期间尤为明显,除燃煤和工业排放外,区域的地形和气候特征也是导致雾-霾的主要因素.2019年2月春节期间对汾渭平原临汾站点的空气质量进行观测.运用电感耦合等离子体质谱仪（ICP-MS）对PM_2.5中的13种元素（Li、Be、Ti、Rb、Sc、Y、La、Ce、Zr、V、Tl、U和Sn）进行分析测定,并结合站点的气象数据,运用聚类分析和后向轨迹等方法,分析了污染物的时空分布与潜在源区贡献.结果表明,观测期间SO₂的平均浓度为58.39 μg ·m^-3,超过了国家环境空气质量标准（GB 3095-2012）24 h一级平均质量浓度限值（50μg ·m^-3）,O₃、NO₂和CO的均值浓度分别为52.15 μg ·m^-3、29.02 μg ·m^-3和2.29 mg ·m^-3.聚类分析结果表明,La、Ce、Ti、V、Li、Be、Rb、Y、U、Sc和Zr主要受地壳土壤源影响.气态污染物的空间分析结果表明SO₂是主要污染物,主要受当地燃煤排放的影响,而高浓度的NO₂和CO主要由城区向观测站点扩散造成.受汾渭平原盆地地形的影响,沿汾渭平原传输的气团一直存在,表明当地的地形可能会限制污染物扩散,加剧雾-霾现象.土壤源的潜在源区分析（PSCF）表明：受季风气候影响,陕西北部、甘肃南部和宁夏南部对站点的土壤扬尘源有主要贡献.     

黄土高原黄土的成因:沙尘气溶胶源汇模拟与黄土堆积

黄土高原是重要的降尘区还是沙尘源区这一科学问题至今未有确切定论.本文利用北半球气溶胶区域气候模式NARCM,根据1995~2004年10a的模拟数据,分析了中国区域沙尘起沙量、沉降量以及沙尘的盈亏空间分布及风场,得到如下结论:1)沙漠及沙漠化地区是起沙量最大的区域、沉降量高值区集中在沙漠、沙漠化地区及其下风方向.黄土高原起沙量很小,而沉降量远大于起沙量.2)沙尘源区是沙漠及沙漠化地区,其余的地区则是沙尘汇区,降尘量由西北向东南递减.3)黄土高原因太行山和秦岭阻挡,处在最大的沙尘汇区.黄土高原的黄土是冰期和间冰期交替、经过漫长年代沙尘沉降的结果,模拟分析结论为黄土的风成学说提供了有力的证据.     

汾渭平原秋冬季PM2.5化学组分特征及其来源

汾渭平原是我国空气污染最严重的区域之一,2018年被列为重点区域. 本研究针对汾渭平原11城市开展PM_2.5化学组分连续观测,分析PM_2.5浓度和主要化学组分的时空分布规律,并利用PMF模型解析PM_2.5污染来源. 结果表明:①2018—2019年秋冬季汾渭平原11城市ρ(PM_2.5)平均值为(101.4±65.4)μg/m3,是京津冀及周边地区“2+26”城市的1.1倍. 临汾市ρ(PM_2.5)最高(216.8 μg/m3),是汾渭平原的2.1倍. ②2018—2019年秋冬季汾渭平原PM_2.5的主要化学组分是有机物、硝酸根离子、地壳物质和硫酸根离子,其中地壳物质占比是京津冀及周边地区的1.6倍. ③受污染物排放、气象条件以及地理位置的影响,汾渭平原PM_2.5中有机物、硝酸根离子、地壳物质、硫酸根离子、铵根离子和氯离子的空间分布具有明显的差异性. ④随着污染的加重,硝酸根离子、硫酸根离子和氯离子在PM_2.5中的占比均逐渐增加,地壳物质、元素碳、微量元素等与一次排放相关的组分占比随污染加重逐渐减少,表明污染期间燃煤源管控仍需进一步加严,而对扬尘源和机动车等污染源的管控起到了良好的效果. ⑤重污染过程期间,相对湿度增加、风速减小是影响PM_2.5浓度上升的客观因素,二次组分以及与燃煤源和生物质燃烧源有关的化学组分的增长是影响PM_2.5浓度上升的重要原因,二次源和燃烧源是PM_2.5的主要来源. 研究显示,汾渭平原秋冬季PM_2.5污染较重,尤其需要关注燃烧源的管控.      

基于CMAQ模式的自适应“nudging”源反演方法的中国主要污染区排放特征分析

中国中东部地区的空气污染主要集中在京津冀、长三角、珠三角、东北地区及汾渭平原等区域，各区域的污染排放特征各异.本文应用基于CMAQ（The Community Multiscale Air Quality）模式的自适应"nudging"源反演方法，反演中国中东部地区2016年12月—2017年1月逐日NO_x污染源，分析上述主要污染区的污染物排放强度空间分布特征，并与2016年MEIC（The Multi-resolution emission inventory for China）排放源进行比较，检验反演源的可靠性.结果表明，2016年冬季各个区域反演源NO_x排放强度空间分布特征与2016年MEIC排放源基本一致.京津冀地区高强度排放区域形成沿山前区域东北-西南走向的NO_x高强度排放带；长三角地区NO_x高强度排放区域位于常州、苏州、上海和湖州等城市构成的城市群；珠三角地区NO_x高强度排放区域位于以广州为中心的大范围城市群且排放强度呈现向四周逐渐降低的放射状分布；东北地区NO_x高强度排放区域空间分布特征呈现以城市为中心且稀疏分布；汾渭平原排放区域呈现以城市为中心且向峡谷中间集中分布，排放区域轮廓与汾渭平原狭长的新月状相符.     

太原市秋冬季大气污染特征和输送路径及潜在源区分析

采用环境空气质量指数(AQI)统计分析了2014～2018年太原市全年及秋冬季污染特征,并采用HYSPLIT后向轨迹模型计算了2014～2017年秋冬季逐时后向轨迹,结合太原市AQI,通过聚类分析、潜在源贡献因子和浓度权重轨迹方法对影响太原市的污染物输送路径和潜在源区进行了分析.结果表明,太原市污染状况不容乐观,太原市2014～2018年全年优良天数波动较大,尤其近两年从64%下降到不足50%;然而秋冬季优良天数稳步上升,2018年超过50%,空气质量有好转趋势.污染类型可能发生变化,全年及秋冬季PM_(2.5)为首要污染物的污染天数下降显著,PM_(10)为首要污染物的天数上升明显.聚类分析2014～2017年秋冬季太原的后向轨迹,53%的气团来自偏西方向,21%来自西北方向,12%来自西南方向,14%来自偏东方向,其中西南方向轨迹是外来污染物输送进入太原的主要轨迹,对太原空气质量有显著影响.PSCF和CWT分析表明,影响太原空气质量的重要潜在源区主要位于汾渭平原的陕西汉中、西安和山西的吕梁、临汾等地.建立汾渭平原及其周边区域联防联控机制对控制区域污染有着重要意义.     

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.     

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.     

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.