大气气溶胶中硝基多环芳烃分析方法的建立及应用

硝基多环芳烃类化合物是一类强致突变和致癌物.大气中的硝基多环芳烃主要由化石类燃料燃烧时直接释放,或由前体化合物多环芳烃经光化学反应生成,其浓度远低于多环芳烃.利用高效液相色谱法,分离并富集目标组分,结合气相色谱-质谱技术,建立大气气溶胶中硝基多环芳烃类化合物的检测方法,仪器检测限为1.17～2.94pg,硝基多环芳烃指...     

底泥中氮杂多环芳烃及硝基多环芳烃的分离与鉴定

本文报道了毛细管柱色谱质谱联用及选择离子检测方法分析鉴定北京东南郊排污河底泥样品中氮杂芳烃及硝基多环芳烃的实验结果.研究了十二种标样的EI谱.样品中鉴定出25种含氮多环芳烃,检测出底泥样品中含有硝基多环芳烃.并讨论了实验结果.     

太原城区PM2.5中多环芳烃、硝基多环芳烃的污染特征、来源解析和健康风险评价

以2013—2014年期间太原城区大气细颗粒物(PM_(2.5))为研究对象,定量分析了其中多环芳烃和硝基多环芳烃的浓度.结果显示,太原城区PM_(2.5)中16种多环芳烃和12种硝基多环芳烃的浓度分别为13.8~547和0.70~4.33 ng·m~(-3),硝基多环芳烃浓度低于多环芳烃浓度1~2个数量级.太原城区PM_(2.5)中多环芳烃最高值出现在冬季,最低值出现在夏季,冬季污染物浓度平均值高于夏季20倍,主要是由于北方采暖期间取暖用煤量的增加使得多环芳烃排放量大幅提高;与之不同的是,硝基多环芳烃浓度季节变化并不显著,冬季浓度均值与夏季差异小于5倍(除9-硝基蒽),反映出硝基多环芳烃生成主要与机动车尾气排放有关,其排放不受季节控制,这与实际情况是吻合的.此外,基于因子分析和化合物比值结果发现,太原城区大气PM_(2.5)中9-硝基蒽有来自周边地区木材燃烧的贡献.健康风险评价结果表明,必须对多环芳烃排放进行有效控制来降低人群在冬季大气中的暴露风险;对于硝基多环芳烃,其健康风险更要引起足够的重视.     

南京市大气细颗粒物(PM2.5)中硝基多环芳烃污染特征与风险评估

硝基多环芳烃是大气细颗粒物中具有致癌效应的一类重要污染物,为探明硝基多环芳烃污染特征与来源,采集南京市14个大气细颗粒样品,利用气相色谱-质谱联用仪（GC-MS）测定硝基多环芳烃浓度,进行分布特征分析,来源识别和健康风险评估.结果表明,南京市大气细颗粒物中2,8-二硝基二苯并噻吩（743 pg·m^-3）、2,7-二硝基芴（331 pg·m^-3）、9-硝基蒽（326 pg·m^-3）、3-硝基荧蒽（217 pg·m^-3）和1,8-二硝基芘（193 pg·m^-3）为主要的硝基多环芳烃;硝基多环芳烃检出浓度具有明显的季节变化,冬季最高（3082 pg·m^-3）,秋季其次（1553 pg·m^-3）,春季最低（1218 pg·m^-3）.南京市大气细颗粒物中硝基多环芳烃主要来自多环芳烃大气光氧化反应与生物质燃烧,二次生成是硝基多环芳烃的重要来源.当前南京PM_2.5中硝基多环芳烃的致癌风险可控,二硝基多环芳烃是致癌风险的主要来源.     

硝基多环芳烃的致突变活性-结构关系研究进展

硝基多环芳烃是一类重要的具有直接致突变性的环境污染物。本文就硝基多环芳烃的致突变性、结构与致突变活性之间的关系方面的研究进展加以综合评述。     

硝基多环芳烃的致突变性理化参数之间的定量结构活性关系

硝基多环芳烃因具有直接致突变性，潜在致癌性以及在环境中的广泛存在而引起人们的关注。本文在硝基多环芳烃的突变活性理化参数之间建立了１０个定量结构活性关系式。并利用溶解度与致突变性之间的结构活性关系对５０种硝基多环芳烃的致突变能力进行预测，正确率达７８％。     

硝基多环芳烃的致突变性与理化参数之间的定量结构活性关系

硝基多环芳烃因具有直接致突变性、潜在致癌性以及在环境中的广泛存在而引起人们的关注。本文在硝基多环芳烃的致突变活性与理化参数（正辛醇－水分配系数、水溶解度、分子连接性指数）之间建立了１０个定量结构活性关系式。并利用溶解度与致突变性之间的结构活性关系对５０种硝基多环芳烃的致突变能力进行预测，正确率达７８％。     

首钢焦化厂环境中多环芳烃分布赋存特征研究

对首钢焦化厂炼焦过程中生成多环芳烃的分布特征进行了初步研究.焦化厂环境中共检测出40多种多环芳烃,其中属于美国国家环保局(EPA)优先控制污染物9种,且大多具有致癌和致突变性.多环芳烃的稳定碳同位素可以初步确定环境颗粒物中PAHs的来源,以及是否混有未燃烧、燃烧不完全或干馏中间产物的颗粒物.研究表明,煤中多环芳烃通过焦化作业以烟尘、煤粒、焦末以及外排废水形式迁移而污染大气、土壤和水环境.     

拉萨市城区大气和拉鲁湿地土壤中的多环芳烃

对拉萨城区大气及郊区湿地土壤中多环芳烃的研究表明,大气中的多环芳烃,颗粒物占27.69%,气相状态占72.31%;由于高原高强度的紫外线辐射,无论是颗粒相还是气相状态存在的多环芳烃含量均是夜晚高于白天;颗粒物中的多环芳烃主要为3个苯环数以上的,而气相状态的多环芳烃多为2和3个苯环数的芳烃及芘.湿地土壤中的多环芳烃主要来自于大气,其中气相状态占52.56%,颗粒物占47.44%.     

北京地区大气可吸入颗粒物中多环芳烃分布特征

采集北京城乡结合区和郊区冬季12个大气可吸入颗粒物不同粒径样品,用色谱-质谱技术分析鉴定了75种多环芳烃化合物,并对各粒径中美国EPA优控的16种多环芳烃做了定量分析,研究其在不同粒径的分布规律。结果表明:城乡结合区大气颗粒物中优控多环芳烃总量明显高于郊区;郊区和城乡结合区大气分别有68%和85%的优控多环芳烃吸附在粒径小于2 0μm颗粒物上;可吸入颗粒物中都相对富集高环数的多环芳烃;2个地区主要污染源可能为化石燃料的燃烧排放,燃煤的影响相对较大。      

Urban and rural transport of semivolatile organic compounds at regional scale: A multimedia model approach

Urban areas are generally regarded as major sources of some semivolatile organic compounds and other persistent organic pollutants(POPs) to the surrounding regions. Huge differences in contaminant emissions between urban and rural areas directly affect their fate in environmental media. Little is known about POPs behavior between urban and rural areas at a regional scale. A spatially resolved Berkeley-Trent-Urban-Rural Fate Model(BETR-UR) was designed by coupling land cover information to simulate the transport of POPs between urban and rural areas, and the Bohai Rim was used as a case study to estimate Polycyclic Aromatic Hydrocarbon(PAH) fate. The processes of contaminant fate including emission, inter-compartmental transfer, advection and degradation in urban and rural areas were simulated in the model. Simulated PAH concentrations in environmental media of urban and rural areas were very close to measured values. The model accuracy was highly improved, with the average absolute relative error for PAH concentrations reduced from 37% to 3% compared with unimproved model results. PAH concentrations in urban soil and air were considerably higher than those in rural areas. Sensitivity analysis showed temperature was the most influential parameter for Phen rather than for Bap, whose fate was more influenced by emission rate, compartment dimension, transport velocity and chemical persistence. Uncertainty analysis indicated modeled results in urban media had higher uncertainty than those in rural areas due to larger variations of emissions in urban areas. The differences in urban and rural areas provided us with valuable guidance on policy setting for urban–rural POP control.     

根据具体情况优化EPA8310中色谱分离条件

运用Agilent（安捷伦）1200系列高效液相色谱和多环芳烃专用柱ZORBAX Eclipse PAH（4.6×250mm、5μm,P.N.959990-918,S.N.USPAB01066）,对16种多环芳烃化合物混合溶液进行分析,根据具体实验条件优化EPA8310中色谱分离条件并得到了更节省时间、分离效率更好的流动相梯度变化程序。     

高效液相色谱测定烟尘中的多环芳烃

本文详细介绍了用高效液相色谱测定烟炱中的多环芳烃的方法和前处理，及有关色谱条件的选择等因素。并对环境中实际样品进行了测定，得到满意的结果。     

Multi-factors influencing the spatial distribution of polycyclic aromatic hydrocarbons in soils surrounding drinking water protection zone

We selected the Guanting Reservoir in Beijing, China as a case where an industrial area locates on the upwind corner to study the influence of human activities and natural processes on the distribution of polycyclic aromatic hydrocarbons (PAHs) in soils. Soil PAH concentrations in the study area follow a log-normal probability distribution function, suggesting that distribution of PAH in soils was affected by human activities. Distribution of PAHs in soils was significantly affected by the point source that high PAH concentrations were observed in near industrial area with an obvious declining trend from the northwest to the southeast which was the prevailing wind direction in this area. Away from the influence of point source, distribution of PAHs in soils was found to significantly correlate with total organic carbon content, while the influences of agricultural land uses and type of soil texture on the total soil PAHs contents and ring compositions were quite limited. The results can provide some evidences and data on the pollutant accumulation in drink water protection area influenced by natural processes and human activities.     

生物堆修复城市多环芳烃污染土壤的调控研究

土壤多环芳烃(PAHs)污染已成为一种严重的全球性城市环境问题。以通风时间、绿肥、无机营养剂和疏松剂含量为调控因素,利用现场规模的正交试验进行了生物堆修复城市多环芳烃污染土壤的调控研究。结果表明,所有生物堆处理对土壤PAHs的去除均有一定促进作用,75 d时平均降解率为30.63%~80.41%,且深层土壤降解率比表层土壤高8.55%;运行期间各调控因素对不同深度土壤PAHs降解的影响程度和作用规律各不相同,其中通风时间始终是主导因素,且通风时间越长,降解效果越好;生物堆的最佳运行条件总体上为通风时间3 h、绿肥3.5%、营养剂0.2%、疏松剂18%(表层土壤)或14%(深层土壤)。因此,利用生物堆修复城市PAHs污染土壤是有效的,且增加通风时间是提高其修复效率的优先调控方式。     

The study for polyaromatic hydrocarbons decay on Chinese coal soot particles in atmosphere

A study for the photochemical behavior of some polyaromatic hydrocarbons (PAH), for example B(a )P, B( k )F and fluoranthene in coal smoke particles was performed by using indoor Teflon smog chamber.Experiments suggest that the photochemical reaction of PAH is first order reaction and kinetic rates of some PAH were obtained. It was shown that the reaction rate constant is proportional to light intensity and water vapor concentration. Temperature and PAH loading also have influence on PAH decay rate. A model for PAH loss has been set up on the basis of the results of our experiments and the simulating results of this model suggest that coal particle PAH half lives are of the order of a period of days in winter and a few hours in summer. Other factors which may have effect on the photochemical reaction of PAH have also been discussed.     

Yangtze Three Gorges Reservoir, China: A holistic assessment of organic pollution, mutagenic effects of sediments and genotoxic impacts on fish

Besides obvious benefits,the Three Gorges Dam's construction resulted in new pollution scenarios with the potentials to threaten the Three Gorges Reservoir(TGR) ecosystem.In order to record organic contamination,to find links to ecotoxicological impacts and to serve as reference for ensuing monitoring,several sites in the TGR area were screened applying the triad approach with additional lines-of-evidence as a holistic assessment method.Sediments and the benthic fish species Pelteobagrus vachellii were sampled in 2011 and 2012 to determine organic pollution levels,mutagenic potentials and genotoxic impacts.Two regional hot-spots near the cities of Chongqing and Kaixian were identified and further investigated in 2013.Only polycyclic aromatic hydrocarbons(PAHs) could be detected in sediments in 2011(165–1653 ng/g),emphasizing their roles as key pollutants of the area.Their ubiquity was confirmed at Chongqing(150–433 ng/g) and Kaixian(127–590 ng/g) in2013.Concentrations were comparable to other major Chinese and German rivers.However,the immense sediment influx suggested a deposition of 216–636 kg PAH/day(0.2–0.6 mg PAH/(m2·day)),indicating an ecotoxicological risk.PAH source analysis highlighted primary impacts of combustion sources on the more industrialized upper TGR section,whereas petrogenic sources dominated the mid-low section.Furthermore,sediment extracts from several sites exhibited significant activities of frameshift promutagens in the Ames fluctuation assay.Additionally,significant genotoxic impairments in erythrocytes of P.vachellii were detected(Chongqing/Kaixian),demonstrating the relevance of genotoxicity as animportant mode of action in the TGR's fish.PAHs,their derivatives and non-target compounds are considered as main causative agents.     

聚酰肼接枝改性活性炭除甲醛材料的制备及其影响因素

为解决甲醛污染问题,开展了多胺高分子接枝活性炭环境材料制备研究.采用质量比为1:1的硫酸和硝酸的混合液对活性炭表面改性,再以DCC（N,N-二环己基碳二亚胺）为胺化反应的缩水剂,通过PAH（聚酰肼）和活性炭缩聚反应制备了除甲醛材料ACm-g-PAH（聚酰肼接枝改性活性炭）,通过单因素试验探讨了影响ACm-g-PAH除甲醛的因素,再由正交试验得出ACm-g-PAH制备的最佳工艺为活化温度为90℃,w（DCC）为2.0%,c（PAH）为12 mmol/L.结果表明:在温度为10~50℃与相对湿度为45%~85%区间内,温度和相对湿度对甲醛去除率影响并不明显.吸附甲醛的ACm-g-PAH经弱酸还原再生技术处理后,再生5次的ACm-g-PAH对甲醛的去除率仍能达到初生材料的89.2%.FTIR（红外光谱）证明了在DCC存在下,聚酰肼高分子PAH与ACm（改性活性炭）表面羧基缩聚反应的事实.随着c（PAH）的增加,SEM（扫描电镜）显示活性炭孔内的PAH呈堆积的现象;TG（热重分析）图谱的测试结果表明,ACm-g-PAH的降解温度在330~420℃之间.研究显示,ACm-g-PAH对甲醛的去除率最高为99.4%.      

杭州市交通道口大气飘尘中多环芳烃的研究

对杭州市某交通道口的可吸入颗粒物 ( IP)浓度进行测定 ,IP浓度为 1 1 2 /ng·m- 3 ,并用 HPLC对其中的多环芳烃进行定性、定量分析 ,鉴定出 1 0种 ,其中 Ba P浓度为 1 0 .51 /ng· m- 3 。     

鞍山市环境空气颗粒物中多环芳烃污染状况分析

采用高效液相色谱测定了鞍山市环境空气中总悬浮颗粒物及降尘中的多环芳烃的污染状况，掌握了鞍山市环境空气颗粒中多环芳烃的污染分布规律，为环境治理和环境规划提供了科学的依据。