山东省空气质量预报平台设计及其预报效果评估

基于排放源处理(SMOKE)模型、综合空气质量(CMAQ)模型与气象预报(WRF)模型初步搭建山东省空气质量预报平台,利用污染物在线监测数据和气象站观测数据检验预报平台的预报效果。结果表明,预报平台气象模块的预测效果与文献研究结果较一致;由CMAQ模型对2014年济南、淄博、烟台、威海的SO2、NO2、PM2.5质量浓度进行预测,SO2、NO2、PM2.5预报平均值分别在17.65~48.97、18.69~45.43、34.97~79.15μg/m3;SO2、NO2、PM2.5预报值与监测值的相关系数在0.52~0.74,标准化平均偏差、标准化平均误差、平均相对偏差、平均相对误差分别在-34.00%~-5.73%、11%~47%、-25.00%~-10.21%、20%~42%,预报平台具有良好的预报性能。最后,对未来空气质量数值预报平台的发展提出建议。     

北京与伦敦空气中气态污染物的比对研究

城市空气质量问题已经引起广泛关注.通过对中英2个大城市北京与伦敦 2004 年 8 月～2005 年12 月空气中气态污染物 O3、NOx、SO2 和 CO 浓度变化的分析与对比发现:参照世界卫生组织空气质最准则、欧盟空气质量标准、美国国家空气质量标准或国家空气质量二级标准,北京O3、NO2、SO2和 CO 浓度的超标天数或时数明显高于伦敦.观测期内,北京 O3、NOx、SO2 和 CO 浓度明显高于伦敦,平均值分别是 17.9±22.1×10-9、72.4±76.1×10-9、19.5±21.8×10-9、2 004.6±1 509.8×10-9与10.8±9.9×10-9、54,6±38.9×10-9、1.8±2.2×10-9、372.3±235.0×10-9.两城市 O3 统计日变化形式均表现为白天高、夜晚低,峰值出现在午后 14:00 左右,日较差分别为 31.5±30.9×10-9与 11.1±7.7×10-9;NO、NO2、SO2 和 CO 呈双峰态日变化,峰值出现在交通的早高峰与晚高峰附近.北京 O3 最高值出现在夏季,而伦敦出现在春季;但两城市NOx、SO2 和 CO 最高值均出现在冬季.北京与伦敦的NO2与 NO 呈显著线性相关,且斜率与截距十分相似,分别是 1.25 和 1.28 与 28.1 和 23.2;同时两城市 CO/NOx 比率明显高于 SO2/NO 分别为 14.0、4.5 与 0.13、0.03.由此可以判断:对于两城市空气污染问题,交通源的贡献要远大于点源;但点源也对两城市空气质量造成影响.此外,连续逆温的天气是造成重污染事件的原因.     

丽水市大气污染的时空分布特征及与气象要素的相关分析

利用2007-2010年丽水市逐日大气污染物浓度数据和地面气象观测资料,对PM10、SO2、NO23种大气污染物浓度进行了时空分布特征研究,进而探讨了气象要素对大气污染的影响.结果表明:2007-2010年,丽水市主要的3种大气污染物的负荷为PM10＞ NO2 ＞SO2,影响大气环境质量的污染物以PM10为主;总体来说,NO2的月均浓度基本达到《环境空气质量标准》(GB3095-1996)-级标准,冬半年(9-12月、1-2月)SO2的月均浓度仅达到二级标准,而夏半年(3-8月)月均浓度基本达到一级标准,PM10的月均浓度都达到二级标准(0.10 mg/m3);在空间分布上,PM10、NO2的年均浓度都表现出东向西逐渐减少的特征,而SO2年均浓度主要体现为南向北递增的特征,3种大气污染物在空间上都表现为在东部缙云、青田等地的污染相对严重,而在西面的遂昌、龙泉等地的污染程度较轻;各种气象要素对大气污染的影响中,除了气压与3种大气污染物的浓度呈极显著正相关外,其他气象要素都表现为负相关,只是影响程度有所差异.气象要素对大气污染的影响不是单一作用的,而是通过多种气象要素相互配合、相互作用、综合反应来产生作用的.     

深圳市区空气污染的人工神经网络预测

利用深圳市2006至2013年的大气污染物监测浓度数据和气象资料,分析深圳市空气质量的逐月分布变化特征。采用Pearson相关分析,选择显著相关因子,分别以BP神经网络和RBF神经网络构建空气质量预测模型,对该市2013年SO2、NO2、PM103种空气污染物的月均值进行预测。实验结果表明,通过Pearson相关分析建立的预测模型有更高的预报精度。BP和RBF 2种网络预测效果都比较理想,对不同污染物的预测精度各有高低。但BP网络的构建和参数优化过程较为复杂且网络训练结果不稳定,而RBF网络构建和训练简单,时间短而结果稳定。在综合性能上,RBF网络用于环境空气污染物浓度的预测具有更强的适用性。     

杭州市区大气能见度变化趋势及其与主要污染物相关性分析

利用2004-2006年地面气象观测资料和同期环境空气质量自动监测数据,分析了杭州市区大气能见度变化趋势及其与主要污染物的相关性.结果表明,杭州市区能见度的日分布特征为14时最好,8时最差;季节变化特征为夏季>春季>秋季>冬季,全年仅7月能见度超过10 km;SO2、NO2、PM10浓度均随能见度增高而逐渐降低;影响能见度的首要因子为相对湿度和PM2.5,能见度与PM2.5浓度具有较好的相关性.     

基于改进型灰色神经网络组合模型的空气质量预测

基于空气质量数据不足及波动较大的情况,将灰色GM（1,1）模型与人工神经网络模型组合并改进,建立改进型灰色神经网络组合模型。利用天津市2001—2008年PM10、SO2和NO2年均值作为原始数据预测2009—2010年PM10、SO2和NO2的浓度以进行模型精度检验,最后利用该模型预测2011—2015年天津市空气质量状况。结果表明,与灰色GM（1,1）模型、传统灰色神经网络组合模型相比,所建立的改进型灰色神经网络组合模型相对模拟误差小,预测结果更为可靠,可以用于空气质量预测。     

冬季西安某人工湖污染物分布特征及其相关性分析

以西安某人工湖为研究对象,在湖体中布设9个采样点,并且在2013.12—2014.1期间采样3次,对其中TN、TP、COD、NH+4-N和NO-3-N等污染物分布及其与叶绿素a浓度的相关性进行了相应的研究。结果表明,湖体中NH+4-N、NO-3-N、TN、TP、COD和叶绿素a的浓度分别为:0.8~1.7 mg/L、1.1~2.9 mg/L、2.5~4.8 mg/L、0.04~0.14 mg/L、20~24.8 mg/L和0.82~2.14μg/L。人工湖进、出水口污染物浓度整体较低,在靠近车流量较大的3座交通桥的采样点4、5和8采样后所测各项污染指标均较其他点高,由此说明在研究期间交通桥可能成为此人工湖的点污染源。污染物相关性分析结果显示,在冬季低温条件下(4~6℃)叶绿素a与TN、TP、NH+4-N、NO-3-N的相关系数分别为:R2=0.55~0.75,P0.05;R2=0.4~0.65,P0.05;R2=0.48~0.62,P0.05;R2=0.15~0.44,P0.05;COD和浊度呈极显著相关:R2=0.67~0.85,P0.01。     

一次光化学污染过程中O_3和NOx的垂直梯度观测研究

为了研究2008年北京奥运会前期污染物浓度变化特征,对北京气象塔3层高度上的大气污染物(NO2和O3)进行加强观测,分析其变化特征。观测结果表明,由于北京奥运会前期采取了严格的空气质量控制措施,NO2浓度相对车辆限行前下降了45.3%,且随着高度递增逐渐降低;O3浓度最大值和日均值有所降低,其最大值出现时间较10年前提前了1~2 h,且有4 h左右处于相对平稳状态。O3浓度峰值主要是受NO2的控制,O3浓度峰值出现时间提前反映出北京大气氧化效率不断提高。对于观测期间出现光化学污染事件,利用同期气象资料和大气污染监测数据分析,发现造成这次大气污染的主要原因是气象因子:地面多处于弱高压场控制中,大气层结稳定,风力较弱(小于2 m/s),并伴随着连续高温、强辐射和低湿。     

萧山区环境空气质量变化及其影响因素分析

利用杭州市萧山区环境空气的监测资料,采用空气综合污染指数、空气污染指数(API)、Daniel趋势检验等评价和分析方法,研究了萧山区"十一五"期间(2005—2010年)环境空气质量的变化趋势及其影响因素。结果显示:(1)PM10是萧山区环境空气中的首要污染物。SO2、PM10浓度以及空气综合污染指数先升高后降低,总体呈现不显著下降趋势,整体环境空气质量在2007年后逐年改善。(2)空气中NO2污染负荷系数逐年上升,NO2/SO2和污染物相关性分析结果表明,萧山区空气污染特征正处于由煤烟型向汽车尾气型转变的初期阶段。(3)萧山区月均API呈现出7-9月4-6月1-3月10-12月的变化特征。(4)在持续快速增长、能源消耗逐年增加的情况下,萧山区环境空气质量的改善说明节能减排、产业升级、污染源综合治理、能源清洁使用等措施对改善环境空气质量起到了关键作用。     

小波分析在郑州市供暖期PM_(2.5)浓度相关性分析中的应用

为分析供暖期内各种物质与PM2.5的相关性和变化规律,以郑州市供暖期为例,运用Morlet小波分别对PM2.5、PM10、CO、NO2、和SO2的浓度进行分析,并对比各自主周期的小波系数模。结果表明,PM10与PM2.5波动主周期均为33 d,主周期小波系数模差值为0,与PM2.5相关性最高;SO2波动主周期为12 d,与PM2.5相差最大,相关性最低。由于燃煤中各成分含量不同,供暖期SO2与CO、NO2呈中度相关,相关系数依次为0.6045和0.6949;SO2与PM10呈低度相关,相关系数为0.4010。供暖期污染最严重的污染物是PM10和NO2,与非供暖期相比,两者与PM2.5相关系数增量分别为:0.1255和0.2858,相关性提高幅度较大。     

Persistence and dissipation kinetics of trifloxystrobin and tebuconazole in onion and soil

The persistence and dissipation kinetics of trifloxystrobin and tebuconazole on onion were studied after application of their combination formulation at a standard and double dose of 75 + 150 and 150 + 300 g a.i. ha^?1. The fungicides were extracted with acetone, cleaned-up using activated charcoal (trifloxystrobin) and neutral alumina (tebuconazole). Analysis was carried out by gas chromatograph (GC) and confirmed by gas chromatograph mass spectrometry (GC-MS). The recovery was above 80% and limit of quantification (LOQ) 0.05 mg kg^?1 for both fungicides. Initial residue deposits of trifloxystrobin were 0.68 and 1.01 mg kg^?1 and tebuconazole 0.673 and 1.95 mg kg^?1 from standard and double dose treatments, respectively. Dissipation of the fungicides followed first-order kinetics and the half life of degradation was 6–6.6 days. Matured onion bulb (and field soil) harvested after 30 days was free from fungicide residues. These findings suggest recommended safe pre-harvest interval (PHI) of 14 and 25 days for spring onion consumption after treatment of Nativo 75 WG at the standard and double doses, respectively. Matured onion bulbs at harvest were free from fungicide residues.     

Sorption and Desorption Behavior of Chloroanilines and Chlorophenols on Montmorillonite and Kaolinite

The bioavailability of pollutants, pesticides and/or their degradation products in soil depends on the strength of their sorption by the different soil components, particularly by the clay minerals. This study reports the sorption-desorption behavior of the environmentally hazardous industrial pollutants and certain pesticides degradation products, 3-chloroaniline, 3,4-dichloroaniline, 2,4,6-trichloroaniline, 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlorophenol on the reference clays kaolinite KGa-1 and Na-montmorillonite SWy-l. In batch studies, 2.0 g of clay were equilibrated with 100.0 mL solutions of each chemical at concentrations ranging from 10.0 to 200.0 mg/L. The uptake of the compounds was deduced from the results of HPLC-UV-Vis analysis. The lipophilic species were best retained by both clay materials. The most lipophilic chemical used in the study, 2,4,6-trichloroaniline, was also the most strongly retained, with sorption of up to 8 mg/g. In desorption experiments, which also relied on HPLC-UV-Vis technique, 2,4,6-trichloroaniline was the least desorbed from montmorillonite. However, on kaolinite all of the compounds under study were irreversibly retained. The experimental data have been modelled according to the Langmuir and Freundlich isotherms. A hypothesis is proposed concerning the sorption mechanism and potential applications of the findings in remediation strategies have been suggested.     

Field and laboratory studies of the fate and enantiomeric enrichment of venlafaxine and O-desmethylvenlafaxine under aerobic and anaerobic conditions

The stereoselectivity of R,S-venlafaxine and its metabolites R,S-O-desmethylvenlafaxine, N-desmethylvenlafaxine, O,N-didesmethylvenlafaxine, N,N-didesmethylvenlafaxine and tridesmethylvenlafaxine was studied in three processes: (i) anaerobic and aerobic laboratory scale tests; (ii) six wastewater treatment plants (WWTPs) operating under different conditions; and (iii) a variety of wastewater treatments including conventional activated sludge, natural attenuation along a receiving river stream and storage in operational and seasonal reservoirs. In the laboratory and field studies, the degradation of the venlafaxine yielded O-desmethylvenalfaxine as the dominant metabolite under aerobic and anaerobic conditions. Venlafaxine was almost exclusively converted to O-desmethylvenlafaxine under anaerobic conditions, but only a fraction of the drug was transformed to O-desmethylvenlafaxine under aerobic conditions. Degradation of venlafaxine involved only small stereoisomeric selectivity. In contrast, the degradation of O-desmethylvenlafaxine yielded remarkable S to R enrichment under aerobic conditions but none under anaerobic conditions. Determination of venlafaxine and its metabolites in the WWTPs agreed well with the stereoselectivity observed in the laboratory studies. Our results suggest that the levels of the drug and its metabolites and the stereoisomeric enrichment of the metabolite and its parent drug can be used for source tracking and for discrimination between domestic and nondomestic wastewater pollution. This was indeed demonstrated in the investigations carried out at the Jerusalem WWTP.     

Synthesis and characterization of m- and p-methylbenzyl-mercapturic acids derived from m- and p-xylenes

Chemical synthesis and physical properties of two mercapturic acids suggested as urinary metabolites of m- and p-xylenes ace described. These compounds may be used for the identification and quantivative determination by high-performance liquid chromatography of the corresponding mercapturic acids in urine.     

Copper-catalyzed chlorination and condensation of acetylene and dichloroacetylene

The chlorination and condensation of acetylene at low temperatures is demonstrated using copper chlorides as chlorinated agents coated to model borosilicate surfaces. Experiments with and without both a chlorine source and borosilicate surfaces indicate the absence of gas-phase and gas-surface reactions. Chlorination and condensation occur only in the presence of the copper catalyst. C₂ through C₈ organic products were observed in the effluent; PCDD/F were only observed from extraction of the borosilicate surfaces. A global reaction model is proposed that is consistent with the observed product distributions. Similar experiments with dichloroacetylene indicate greater reactivity in the absence of the copper catalyst. Reaction is observed in the gas-phase and in the presence of borosilicate surfaces at low temperatures. The formation of hexachlorobenzene is only observed in the presence of a copper catalyst. PCDD/F were only observed from extraction of the borosilicate surfaces. A global reaction model is proposed for the formation of hexachlorobenzene from dichloroacetylene.     

Aerobic and anaerobic degradation of profluralin and trifluralin

Abstract

The degradation of profluralin [N‐(cyclopropylmethyl)‐α,α,α‐trifluoro‐2,6‐dinitro‐N‐propyl‐]p‐toluidine] and trifluralin (α,α,α‐trifluoro‐2,6‐dinitro‐N,N‐dipropyl‐p‐toluidine) was studied under aerobic and anaerobic soil conditions. Three soils (Goldsboro loamy sand, Cecil loamy sand, Drummer clay loam) were each treated with 1 ppmw herbicide; anaerobic conditions were maintained by flooding. Soil samples were extracted monthly and subjected to TLC analysis. No degradation was detected in sterile controls. Aerobic degradation of both herbicides was greatest in the Cecil loamy sand soil over the entire incubation period. Degradation of profluralin in Cecil soil under aerobic conditions was 86 percent after 4 months with three products detected; 83 percent of the trifluralin was degraded with two products detected. Anaerobic degradation accounted for 72 percent of the profluralin and 78 percent of the trifluralin after 4 months. Degradation of both herbicides increased with incubation time for the first 3 months and decreased slightly thereafter. Generally there was more extensive degradation (percent and in number of products formed) of profluralin than trifluralin under the conditions tested. More degradation products were detected for both herbicides under aerobic conditions than under anaerobic conditions.     

Levels of PCDDs and PCDFs in products and effluent from the Swedish pulp and paper industry and chloralkali process

Within the Swedish Dioxin Survey various samples from the pulp and paper industry and the chloralkali process have been analyzed by congener specific analytical methods. In addition to the generally discussed “bleaching pattern” of the tetrachlorinated congeners, these samples also contained higher chlorinated congeners like hexa-CDDs, hepta-CDFs, octa-CDD and octa-CDF. Consequently it is recommended that samples from the pulp industry should be analyzed for all PCDDs and PCDFs (tetra- through octa-). Counted as Nordic Toxic Equivalents (NTEQ), the recycled pulp samples had the highest contamination level followed by TMP, unbleached sulfite and bleached softwood and hardwood. In addition to the bleaching process, various chemicals used in the pulping, bleaching and wastewater treatment can contribute to the contamination.     

Uptake and translocation of metformin, ciprofloxacin and narasin in forage- and crop plants

Transfer of bioactive organic compounds from soil to plants might represent animal and human health risks. Sewage sludge and manure are potential sources for bioactive compounds such as human- and veterinary drugs. In the present study, uptake of the anti-diabetic compound, metformin, the antibiotic agent ciprofloxacin and the anti-coccidial narasin in carrot (Daucuscarota ssp. sativus cvs. Napoli) and barley (Hordeumvulgare) were investigated. The pharmaceuticals were selected in order to cover various chemical properties, in addition to their presence in relevant environmental matrixes. The root concentration factors (RCF) found in the present study were higher than the corresponding leaf concentration factors (LCF) for the three test pharmaceuticals. The uptake of metformin was higher compared with ciprofloxacin and narasin for all plant compartments analyzed. Metformin was studied more explicitly with regard to uptake and translocation in meadow fescue (Festucapratense), three other carrot cultivars (D.carota ssp. sativus cvs. Amager, Rothild and Nutri Red), wheat cereal (Triticumaestivum) and turnip rape seed (Brassicacampestris). Uptake of metformin in meadow fescue was comparable with uptake in the four carrot cultivars (RCF 2-10, LCF approximately 1.5), uptake in wheat cereals were comparable with barley cereals (seed concentration factors, SCF, 0.02-0.04) while the accumulation in turnip rape seeds was as high as 1.5. All three pharmaceuticals produced negative effects on growth and development of carrots when grown in soil concentration of 6-10 mg kg⁻¹ dry weight.     

Sorption and desorption of Cu and Cd by macroalgae and microalgae

The sorption and desorption of Cu and Cd by two species of brown macroalgae and five species of microalgae were studied. The two brown macroalgae, Laminaria japonica and Sargassum kjellmanianum, were found to have high capacities at pHs between 4.0 and 5.0 while for microalgae, optimum pH lay at 6.7. The presence of other cations in solution was found to reduce the sorption of the target cation, suggesting a competition for sorption sites on organisms. Sorption isotherms obeyed the Freundlich equation, suggesting involvement of a multiplicity of mechanisms and sorption sites. For the microalgae tested, Spirulina platensis had the highest capacity for Cd, followed by Nannochloropsis oculata, Phaeodactylum tricornutum, Platymonas cordifolia and Chaetoceros minutissimus. The reversibility of metal sorption by macroalgae was examined and the results show that both HCl and EDTA solutions were very effective in desorbing sorbed metal ions from macroalgae, with up to 99.5% of metals being recovered. The regenerated biomass showed undiminished sorption performance for the two metals studied, suggesting the potential of such material for use in water and wastewater treatment.     

新型高效氧化偶合絮凝剂COF-I的研制及其应用研究

以硫酸铝为主要原料 ,经过化学改性后 ,制得兼具氧化和絮凝为一体的新型、高效水处理药剂COF I ,并设计正交实验找出了药剂最佳组合配方 ,且对微污染水源水、城市污水及印染废水进行了强化处理试验研究。结果表明 ,最佳配方为复合比 1∶1、添加剂含量 1 2 5 %、稳定剂含量 0 3%、氧化成分含量 1 0 % ,在最佳配方和最佳工艺条件下 ,复合药剂COF I对微污染水源水、城市污水及印染废水均具有良好的处理效果