基于气溶胶三维变分同化天津PM2.5数值预报研究

基于气溶胶三维变分同化技术,建立天津空气质量数值模式气溶胶同化模块,通过天津地区两次重污染过程同化模拟敏感性试验,分析了观测资料范围对同化结果的影响,并结合一个月的滚动预报试验,分析了气溶胶同化对天津地区PM_2.5数值预报效果的影响,以期为提升天津空气质量预报能力提供支撑.结果表明：气溶胶同化各控制变量背景误差水平相关系数的衰减尺度约50km,垂直方向上400m高度与模式底层的相关系数衰减至0.6左右;观测资料范围对同化结果影响显著,仅采用天津地区观测数据进行同化,对重污染过程期间天津地区PM_2.5浓度模拟的影响时效约12h,采用模拟区域内所有观测数据进行同化影响时效可持续24h以上,且模拟效果更优;采用三维变分同化技术,实现地面PM_2.5观测资料同化,天津地区PM_2.5数值预报效果显著提升,预报值和实况值之间的相关系数由0.74增加到0.87,均方根误差由32.3μg/m³减小为22.4μg/m³,平均相对误差由39.9%减小为27.1%;同化对模式初始时刻的改进效果最明显,随时间同化效果衰减,14h内改进效果最佳,对24h PM_2.5浓度预报也有明显改进.     

基于GTWR-XGBoost模型的四川省PM2.5小时浓度估算

卫星气溶胶光学厚度(AOD)和气象数据已被广泛用于估算空气动力学直径≤2.5μm的地表颗粒物(PM_2.5)浓度.研究高时间分辨率、高精度的PM_2.5浓度估算方法,对及时准确的空气质量预报和大气污染的预防及缓解具有重要意义.使用Himawari-8 AOD小时产品和ERA5气象再分析资料作为估算变量,提出GTWR-XGBoost组合模型,对四川省PM_2.5小时浓度进行估算.结果表明：(1)提出的组合模型运用于全数据集的性能优于KNN、 RF、 AdaBoost、 GTWR、 GTWR-KNN、 GTWR-RF和GTWR-AdaBoost模型,拟合精度指标R²、 MAE和RMSE分别为0.96、 3.43μg·m^-3和5.52μg·m^-3,验证精度指标R²、 MAE和RMSE分别为0.9、 4.98μg·m^-3和7.92μg·m^-3.(2)该模型作用于PM_2.5浓度小时估算...     

运城市PM2.5时空分布特征和潜在源区季节分析

基于2019年3月～2020年2月环境空气质量监测数据,分析了运城市PM_2.5污染的时空分布特征,并利用HYSPLIT后向轨迹模型和聚类分析等方法探讨不同季节运城市PM_2.5污染的输送路径和潜在源区.结果表明,运城市ρ(PM_2.5)冬季最高(111.24μg·m^-3),夏季最低(30.02μg·m^-3),PM_2.5/PM₁₀秋冬季均大于0.6,表明运城市秋冬两季颗粒物污染以细颗粒物为主;空间上ρ(PM_2.5)年均值呈现北部和中部高、东部和西部低的分布特征,高值区PM_2.5与SO₂、 NO₂和CO呈显著强相关,表明本地排放对高值区ρ(PM_2.5)影响较大,春季和冬季最高值分别位于河津市(58.50μg·m^-3)和稷山县(142.33μg·m^-3),夏季最高值位于南部的平陆县(36.92...     

冬奥会期间京津冀及周边区域空气质量时空特征、气象影响和减排效果评估

对比分析2015～2022年冬奥会期间(1月31日至2月20日)京津冀及周边区域44城市空气质量时空演变特征,量化同期气象、协同减排和跨区域传输对PM_2.5浓度及组分变化贡献,为不利气象条件下区域空气质量联防联控提供科学参考.结果表明,2022年44城市PM_2.5浓度为近8年农历同期最低(46μg·m^-3),优良天占比最高(83.3%),不存在重污染天.PM_2.5污染南重北轻,高值区主要集中在太行山沿线及燕山传输通道城市.2016年在春节中期未管控烟花爆竹燃放等源排放强度下,优良天占比93.5%,大气强扩散能力对空气质量改善至关重要.2022年静稳天气指数(SWI)同比增加2.1,大气扩散能力转差,44城市ρ(PM_2.5)均值和峰值同比下降14μg·m^-3和76μg·m^-3,北京减排对PM_2.5浓度降幅较未采取前增大96%,晋鲁豫地区在气象造成PM_2.5浓度上升的不利背景下,峰值下降87μg...     

2015~2019年南京北郊碳质气溶胶组成变化

碳质气溶胶是大气细颗粒物的重要组成,对空气质量、人体健康和气候变化有着重要影响.为了探究碳质气溶胶在减排背景下的长期变化,本研究测定了南京北郊5 a（2014年12月17日至2020年1月5日） PM_2.5样品的有机碳（OC）和元素碳（EC）浓度.结果表明,ρ（OC）和ρ（EC）5a平均值分别为（10.2±5.3）μg·m^-3和（1.6±1.1）μg·m^-3,其中OC占PM_2.5的31.1%,EC占PM_2.5的5.2%.OC和EC均呈现出冬高夏低的季节特征.通过非参数的Mann-Kendall检验和Sen’s斜率发现,OC和PM_2.5的浓度整体呈显著下降趋势[OC:P<0.000 1,-0.79μg·（m³·a）^-1,-0.29%·a^-1; PM_2.5:P<0.000 1,-4.59μg·（m³·a）^-1,-1.5...     

南京地区细颗粒物污染输送影响及潜在源区

基于南京市空气质量数据和NCEP全球再分析资料,利用后向轨迹模式计算了2019年3月至2020年2月以南京城区为受体点的逐小时气团24 h后向轨迹,并将后向轨迹数据和PM_2.5浓度数据结合,进行轨迹聚类和潜在源区分析.结果表明,研究期间南京市ρ(PM_2.5)平均值为(36±20)μg·m^-3,超过国家二级标准限值的污染天数为17 d,ρ(PM_2.5)的季节变化特征明显：冬季(49μg·m^-3)>春季(42μg·m^-3)>秋季(31μg·m^-3)>夏季(24μg·m^-3),全年PM_2.5浓度和地面气压显著正相关,而跟气温、相对湿度、降水量和风速均为显著负相关关系;春季气团输送路径为7条,其余季节均为6条,其中,春季的西北路和东南偏南路,秋季东南路和冬季西南路是各季主要的污染输送路径,均具有传输距离短,气团移动慢的特点,说明静稳天气下本地累积是PM_2.5出...     

黄石市大气PM2.5中碳氮组分的污染特征及来源解析

基于稳定同位素技术与正定矩阵因子分解(PMF)模型,探究黄石市城区大气PM_2.5中碳氮组分的污染特征和来源.结果表明,黄石市城区大气PM_2.5中总碳浓度[ρ(TC)]与总碳同位素组成(δ¹³C_TC)均呈冬高夏低的季节性变化特征,夏季分别为(4.4±1.2)μg·m^-3和(-26.3±0.5)‰,冬季分别为(9.9±3.5)μg·m^-3和(-25.5±0.5)‰;总氮浓度[ρ(TN)]在夏季[(9.1±9.1)μg·m^-3]明显低于冬季[(62.4±26.4)μg·m^-3],而总氮同位素组成(δ¹⁵N_TN)在夏季[(12.8±1.9)‰]较冬季[(2.9±4.0)‰]明显富集.除本地源贡献外,黄石市PM_2.5中碳氮组分主要受湖南北部近距离区域排放和西北方向远距离传输影响.贝叶斯混合模型(MixSIAR)与PMF模型解析出机动车排放源为PM_2...     

超低排放改造推广及NH3减排对京津冀冬季环境效益研究

为量化京津冀（BTH）地区超低排放（ULE）改造推广应用潜在的环境效益,基于GEOS-Chem大气化学模型,设计了2个全国情景和6个区域情景,从区域大气输送、超低排放改造在燃煤电厂（CPPs）、工业燃煤（ICB）推广及控制NH₃排放等方面进行研究.结果表明：（1）全国燃煤电厂完成ULE改造,使得京津冀地区2015年1月PM_2.5浓度下降3.2%(2.4μg·m^-3),如只是京津冀地区燃煤电厂完成ULE改造,可使京津冀地区PM_2.5浓度降低1.1%(0.8μg·m^-3),可知区域联防联控对雾霾的治理具有重要意义;（2）在京津冀地区燃煤电厂完成ULE改造的基础上,工业燃煤完成ULE改造、NH₃排放减少30%和50%,可使得京津冀地区PM_2.5浓度分别降低5.4%(3.5μg·m^-3)、4.7%(4.0μg·m^-3)和7.7%(5.7μg·m^-3),可知工业燃煤的ULE改造和...     

重庆典型城区冬季碳质气溶胶的污染特征及来源解析

于2021年1～2月在重庆典型城区万州区(WZ)、渝北区(YB)和双桥区(SQ)同步采集PM_2.5样品,分析冬季碳质气溶胶的污染特征、来源及潜在源区.结果表明,观测期间SQ的ρ(PM_2.5)、ρ(OC)和ρ(EC)均值分别为(72.6±33.3)、(18.2±8.2)和(4.4±1.7)μg·m^-3,高于WZ[(67.2±30.3)、(17.2±7.4)和(5.1±2.4)μg·m^-3]和YB[(63.4±25.7)、(15.4±6.3)和(4.2±1.9)μg·m^-3].与清洁日相比,WZ污染日EC浓度及其对总碳的贡献率均涨幅最大(103.0%和8.1%),但OC/EC值下降最明显(-10.5%),表明WZ污染日碳质气溶胶的一次排放明显增强.观测期间SQ和YB的ρ(SOC)均值分别为(7.7±4.8)μg·m^-3和(6.9±2.8)μg·m^-3,明显高于WZ[(4.5±1.9)μg·m^-3],表明二次转化对SQ...     

焦化行业高污染排放对中国空气质量的影响

为了解焦化行业对中国大气的影响,以地级市为单位收集产焦量等活动水平数据,采用排放因子法建立了我国2020年焦化行业大气污染物的排放清单,并对2021年焦炭产量在1000万t及以上的省份焦化区和非焦化区6种常规污染物的浓度、超标率、作为首要污染物出现的频率和空气质量指数等情况进行了对比分析.结果显示,焦化行业大气污染物的高排放区主要集中在我国山西、陕西、河北、内蒙古、山东等省份(自治区),陕西省榆林市排放量最高.焦化区PM_2.5和PM₁₀的年均浓度(37.7μg·m^-3和82.7μg·m^-3)、超标率(9.78%和9.26%)和作为首要污染物出现的频率(17.82%和35.97%)均高于非焦化区的年均浓度(32.0μg·m^-3和64.6μg·m^-3)、超标率(7.46%和6.74%)和作为首要污染物出现的频率(17.00%和22.33%),SO₂在两个地区均未超标,O₃仅在焦化区的夏季超标,而NO₂     

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.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

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.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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