武汉市2014-2017年大气污染物分布特征及其潜在来源分析

利用武汉市2014—2017年大气污染物（SO₂、NO₂、CO、O₃、PM_2.5和PM₁₀）和气象要素的观测数据,分析了大气污染物的变化特征及其影响因素.使用HYSPLIT模式计算了影响武汉市的主要气团类型,并利用潜在源区贡献（PSCF）和浓度权重轨迹（CWT）分析方法,揭示了研究期内武汉市不同大气污染物的潜在源区分布及其贡献特性.结果表明,武汉市2014—2017年空气质量逐年好转,SO₂、O₃、PM_2.5和PM₁₀的浓度呈逐年下降的趋势,但NO₂和CO的浓度先下降后上升.2017年SO₂、O₃、PM_2.5、PM₁₀、NO₂和CO的浓度分别为9.6、50.8、52.7、89.2、47.5 μg·m^-3和1.1 mg·m^-3,分别比2014年降低了64.3%、23.0%、24.7%、18.8%、3.5%和5.9%.大气污染物存在显著的季节变化和月变化.大气污染物在四个季节中日变化类似,SO₂和O₃均为单峰型分布,NO₂、CO、PM_2.5和PM₁₀均为双峰型分布.武汉市空气污染以PM_2.5为主,随着污染程度的加剧PM_2.5/PM₁₀的值逐渐增大,在空气质量为严重污染时,PM_2.5/PM₁₀高达90%,比空气质量为优时高了31.34%.局地气团（45%）和来自山西、陕西和河南一带的西北气团（12.1%）下大气污染物浓度较高.大气污染物的潜在源区贡献（WPSCF）和浓度权重轨迹（WCWT）的较大值主要集中在武汉市本地及其周边地区,局地污染对武汉市大气污染物的贡献较大,但不同大气污染物受到排放源分布和停留时间等影响其WPSCF和WCWT的分布范围不同.     

基于土地利用回归模型的北京市2013-2019年大气污染时空变化分析

在近年来大力控制大气污染的背景下,通过历史观测数据分析污染物的时空变化特征,有助于总结以往控制的成效,并为制定下一阶段措施提供科学依据.本研究基于北京市大气环境质量监测站点2013—2019年数据,分析了6种常规大气污染物（PM_2.5、NO₂、O₃、PM₁₀、SO₂、CO）的时间变化趋势,并构建了2013和2019年PM_2.5、NO₂和O₃ 3种主要污染物的土地利用回归模型（Land use regression model, LUR）,对它们详细的空间分布及变化特征进行了分析.结果表明,污染物浓度在过去7年中发生了重大变化,除O₃增长,其余5种污染物下降明显.不同城区间的差异在迅速缩小,污染物浓度在空间上趋于均匀.PM_2.5呈明显的南高北低,城区NO₂浓度显著高于郊区和山区,O₃在主城区尤其是道路附近浓度较低.约50%的区域PM_2.5下降30 μg·m^-3以上,约40%的区域NO₂下降幅度为5~15 μg·m^-3,道路附近O₃升幅在20 μg·m^-3以内.研究结果揭示出北京市及其周边地区大气污染治理近年来取得了卓有成效的成绩,但同时也面临着O₃浓度升高的新挑战.     

秦巴山地西部地区2015—2018年大气污染物变化特征及潜在来源分析

为了研究我国南北过渡带西部地区大气污染物变化特征，选取了秦巴山地西部陇南市2015-2018年大气主要污染物监测资料和气象数据，分析了各污染物的浓度水平、变化特征及与气象条件的关系，并利用HYSPLIT后向轨迹模式分析了该地区污染物潜在来源（WPSCF和WCWT）.结果表明：4年来，秦巴山地西部地区空气环境质量较好，空气质量优良率达94.24%，6项大气污染物SO₂、NO₂、CO、O₃、PM_2.5、PM₁₀平均浓度分别为19.02、23.35、701.41、83.11、30.57、56.50 μg·m^-3，均未超过国家二级标准.PM₁₀是该地区首要污染物中天数最多的，达94 d.污染物SO₂、NO₂、CO、PM_2.5和PM₁₀的季节变化和日变化特征具有较好一致性，呈"U"型变化，O₃呈单峰型，在夏季和午后浓度到达高值.颗粒污染物PM₁₀、PM_2.5与气态污染物SO₂、NO₂、CO均呈现较好正相关，气温、降水量和风速风向对污染物浓度有较大的影响.该地区冬季空气质量明显差于其他季节，颗粒物浓度主要受供暖期化石燃料燃烧和外来气流的影响.     

2020年初疫情管控对山东省空气质量影响的模拟

利用2020年初新冠疫情对人类生产、生活的一次自然冲击及由此导致的大气污染状况变化,研究了空气质量对污染物减排及气象因素的响应关系.通过对疫情管控前（1月15~23日）和疫情控制关键期（1月24日~2月7日）这2个阶段空气质量对比分析发现,疫情期间山东省除O₃浓度上升外,PM₁₀、PM_2.5、NO₂、SO₂及CO浓度分别降低72.6 μg·m^-3、47.4 μg·m^-3、25.6 μg·m^-3、3.0 μg·m^-3和0.5 mg·m^-3;降幅分别为45.86%、41.24%、58.00%、17.71%和31.40%;RAMS-CMAQ模拟显示,疫情期气象扩散条件改善导致的PM₁₀、PM_2.5、NO₂、SO₂和CO浓度改善幅度为26.04%、33.03%、28.35%、43.27%和23.29%,人为减排造成的各污染物浓度降低幅度为19.82%、8.21%、29.65%、-25.56%和8.12%.疫情期间O₃浓度上升20.51%,气象因素和人为活动的影响分别占10.47%和10.04%.结果表明一次污染物对减排响应更敏感,二次污染物对减排响应有一定时滞性且受气象因素影响更显著,臭氧浓度对污染物减排线性响应关系不明显,总体呈负相关,说明臭氧的控制需探索科学的污染物减排比例.     

2015—2017年天水市大气污染物变化特征及来源分析

据天水市2015-2017年大气污染物（SO₂、NO₂、CO、O₃、PM_2.5和PM₁₀）的监测数据及气象资料,分析了天水市大气污染物的浓度变化特征,并利用排放源清单和HYSPLIT模型对污染物来源进行了解析.结果表明：①天水市空气质量有所下降,总体优良率达84.9%.SO₂、NO₂、CO均达标,污染物以颗粒物和O₃为主.②一次污染物SO₂、NO₂、CO、PM_2.5和PM₁₀浓度具有相似的季节变化和日变化特征,冬季最高,夏季最低,日变化呈早晚双峰型.二次污染物O₃夏季浓度最高,冬季最低,日变化呈单峰型.③天水市空气质量主要受污染物的本地排放和外来输送的影响,本地民用和工业部门对SO₂、CO、PM_2.5和PM₁₀的贡献最大,交通和工业部门对NO_x的分担率最高,民用部门是CO的最大排放源;西北和东部气流是污染物外来的最主要输送路径.此外,污染物在城市大气中的稀释、扩散和转移也受当地气象因素（气温、降水、风向等）的影响.     

珠江三角洲大气光化学氧化剂(Ox)与PM2.5复合超标污染特征及气象影响因素

基于粤港澳珠江三角洲区域空气监测网络12个监测子站的大气污染物数据,梳理2013~2017年大气光化学氧化剂O_x（NO₂+O₃）与PM_2.5质量浓度的变化趋势.O_x+PM_2.5复合超标污染定义为NO₂和PM_2.5质量浓度日平均值以及O₃浓度日最大8 h平均值（O₃ MDA8）同时超过二级浓度限值,分析了不同类型站点复合超标污染的时空分布特征以及气象因素影响.结果表明,2013~2017年珠三角PM_2.5年均质量浓度由（44±7）μg·m^-3下降至（32±4）μg·m^-3,实现PM_2.5连续3 a达标.O_x年均质量浓度由2013年（127±14）μg·m^-3下降至2016年（114±12）μg·m^-3,2017年反弹至（129±13）μg·m^-3,O₃浓度上升明显（10 μg·m^-3）.以O₃为首要污染物的污染过程占比由2013年33%增多至2017年78%,多个城市同时发生污染的区域特征明显.研究时段内O_x+PM_2.5复合超标污染事件共发生60次,主要在城区站点（78%）和郊区站点（22%）.秋季发生复合超标污染天数最多（52%）,是因为强太阳辐射有利于臭氧生成,大气氧化性增加,进而促进了PM_2.5二次生成.造成珠三角复合超标污染的天气形势主要为高压出海型（43%）、高压控制型（30%）和热带低压型（27%）.就具体气象因素而言,气温在20~25℃且相对湿度在60%~75%的范围内时,复合超标污染事件发生占比最高（22%）.在O₃重污染过程中,夜间高湿和低风速使得NO₂和PM_2.5浓度显著上升,日间高温加剧了复合超标污染.     

2013年中国海域船舶大气污染物排放对空气质量的影响

基于2013年中国海域船舶排放清单和空气质量数值模拟平台（WRF-SMOKE-CMAQ）,利用敏感性分析方法定量识别了中国海域船舶排放对沿海地区空气质量的影响特征. 结果表明：船舶排放对不同污染物的贡献特征空间差异显著,就SO₂、NO₂和PM_2.5而言,在沿海省份的年均贡献率分别为5%、7%、2%（1.1、1.7、0.9 μg·m^-3）,其中,珠三角和长三角地区受影响较大,SO₂、NO₂和PM_2.5贡献分别可达30%、31%、8%（7.7、9.2、2.7 μg·m^-3）和14%、13%、4%（3.7、5.3、1.9 μg·m^-3）.其次,船舶排放对空气质量影响季节性差异显著,尤其表现在PM_2.5的空间分布上,三大城市群中,船舶排放对污染物贡献的季节间最大差异倍数为SO₂（1.3~2.0）,NO₂（1.2~4.0）,PM_2.5（1.8~7.5）.值得关注的是,船舶排放对PM_2.5的浓度贡献表现出了明显的区域性（长距离传输）和复合性.本研究结果,一方面弥补了我国船舶排放对空气质量影响的量化特征认识不足,另一方面可为后续船舶排放的健康影响及控制费效分析等评估研究提供数据支撑.     

典型石化企业排放空气质量影响模拟研究

基于惠州市大亚湾区2017年大气污染源排放清单,利用WRF-CMAQ模型系统量化评估了大亚湾区某典型石化企业在关停和增产排放情景下对周边空气质量的影响.清单结果显示该企业2017年SO₂、NO_x、PM₁₀、PM_2.5、CO和VOCs的排放量分别为212 、1744 、455 、359 、1458 和6446 t,在严格落实等量替代及减排措施后,该石化企业虽然产能翻倍,但VOCs排放量同比2017年显著减少了30%,其它污染物排放量增加了6%~19%.模拟结果显示2017年该石化企业排放对大亚湾区NO₂、PM₁₀、PM_2.5和O₃的浓度贡献分别为0.91、0.64、0.54和-0.08 μg·m^-3,完全关闭该企业排放后对周边站点NO₂改善效果最大（可使邻近管委会子站NO₂浓度下降1.24 μg·m^-3,下降百分比为5.10%）,但由于NO的滴定效应,该企业NO_x减排对周边管委会子站和霞涌子站的O₃浓度均有轻微负贡献;该石化企业的增产改造对周边O₃浓度降低影响明显,周边站点中O₃浓度最高可下降2.45 μg·m^-3（下降幅度为1.72%）,大亚湾区O₃浓度整体也可下降1.45 μg·m^-3.此外,受秋冬季不利扩散条件以及主导上风向污染传输影响,该企业在1月和10月对管委会子站NO₂、PM₁₀和PM_2.5的浓度贡献较大,由于冬季低温导致光化学反应自由基活性降低,该企业在1月对管委会子站O₃浓度负贡献显著.     

厦门湾空气质量对新冠疫情管控的响应

通过对厦门湾城市群在COVID-19封锁前后6周内（2020-01-11~2020-02-21）的空气污染物浓度变化进行分析,以确定影响本区域空气质量的主要人为污染源.在春节假期与封锁叠加期间,SO₂、NO₂、CO、PM₁₀和PM_2.5浓度相比于节前1周的下降幅度分别为6%~22%、53%~70%、34%~48%、47%~64%和53%~60%,而O₃浓度变化没有一致的规律性;与2018~2019年历史同期相比,PM_2.5、PM₁₀、CO和NO₂的下降幅度更大,但SO₂的下降幅度相当;在复工复产后,NO₂的反弹幅度最大（38%~138%）,远高于SO₂（2%~42%）,显示交通源相对于固定源更易受到疫情管控的影响;春节后风速增大和降水增多也为SO₂、NO₂和PM的下降提供了正向影响.利用反距离插值权重法,得到管控前后厦门湾城市群不同污染物的空间分布变化特征,显示NO₂浓度高值区的变化与交通源高度相关,CO和SO₂空间分布特征保持稳定,复工后PM_2.5和PM₁₀在人口与路网密集区变化不明显,而在工地相对集中区域有明显上升,O₃空间分布的低值区与NO₂的高值区具有较好的空间匹配性,显示NO₂对O₃滴定作用明显,可为进一步O₃污染减排措施的制定提供参考.     

上海市大气污染对感冒疾病相对危险度的影响

探讨上海市主要大气污染PM₁₀、PM_2.5、NO₂和O₃的日平均浓度变化以及上海市大气污染对感冒疾病的影响.本文汇总了2008年1月1日~2010年12月31日上海市大气污染、气象要素,以及感冒日就诊人数数据,采用时间序列的Possion半参数广义相加模型,通过平滑样条函数控制长期趋势、"星期几效应"及气象因素等混杂因素的影响,分析上海市大气污染物与居民健康的暴露-反应关系,并按年龄进行分层分析,定量评估上海市大气污染对感冒日就诊人数的影响及滞后效应.结果表明,上海市大气污染物PM₁₀、NO₂、O₃、PM_2.5浓度每增加一个IQR,感冒疾病发生的相对危险度为1.0240（1.0233~1.0246）、1.0206（1.0201~1.0212）、0.9393（0.9384~0.9402）、1.0080（1.0069~1.0086）,大气污染物PM₁₀、NO₂、O₃、PM_2.5浓度每增加10 μg·m^-3,感冒日就诊人数分别增加0.5%、1.0%、-2.0%、0.2%.在多污染模型中,在引入其他污染物后,NO₂和PM_2.5的结果较单污染模型是基本减小的,PM₁₀和O₃的结果是基本增大的.上海市大气污染对感冒疾病的发生有影响.     

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.