Size distribution and diffuse pollution impacts of PAHs in street dust in urban streams in the Yangtze River Delta

Particles of dust washed off streets by stormwater are an important pathway of polyaromatic hydrocarbons (PAHs) into urban streams.This paper presents a comprehensive assessment of the size distribution of PAHs in street dust particles, the potential risks of the particles in urban streams, and the sources and sinks of PAHs in the stream network.This assessment is based on measurements of 16 PAHs from the USEPA priority list in street dust particles and river sediments in Xincheng, China.The content of total PAHs ranged from 1,629 to 8,986 μg/kg in street dust particles, where smaller particles have a higher concentrations.Approximately 55% of the total PAHs were associated with particles less than 250 μm which accounted for 40% of the total mass of street dust.The PAH quantities increased from 2.41 to 46.86 μg/m2 in the sequence of new residential, rising through main roads, old town residential, commercial and industrial areas.The sediments in stream reaches in town were found to be sinks for street dust particle PAHs.The research findings suggest that particle size, land use and the hydrological conditions in the stream network were the factors which most influenced the total loads of PAH in the receiving water bodies.     

贵阳市不同粒级地表灰尘中As、Ni水平及权重

根据贵阳市城区土地利用的情况,在不同功能区地表采集灰尘样品,分析As、Ni含量及变异规律。结果表明:贵阳市地表灰尘As、Ni含量分别为17.4mg/kg和50.0mg/kg。工业区地表灰尘中As、Ni含量最高,商贸区和校园等区域As、Ni水平较低。贵阳市地表灰尘中不同颗粒物的质量百分比大小为细颗粒(<105μm)>中等颗粒(105～250μm)>粗颗粒(250～425μm)。As在不同粒径灰尘中含量差别不大,Ni在不同粒径灰尘中含量随粒径增加而降低。细颗粒对灰尘As、Ni的贡献分别为42%和47%。除垃圾站外,贵阳市各功能区地表灰尘不同粒径颗粒物百分比随粒径增大而减小,其中交通区地表灰尘细颗粒所占比例最大。垃圾站地表灰尘中不同粒径颗粒百分比则随粒径增大而增大,As、Ni在垃圾站地表灰尘中颗粒物贡献为中等颗粒>粗颗粒>细颗粒,其余功能区不同粒径颗粒物的贡献基本为细颗粒大于粗颗粒。     

安徽省室内降尘中多环芳烃分布及来源解析

采集安徽省内14个采样点的24个室内降尘样品,检测16种多环芳烃(PAHs)含量.结果表明,安徽省不同区域室内降尘中ΣPAHs浓度范围为0.52~89.3 μg/g,平均浓度为20.7 μg/g.降尘中PAHs以5环为主,其次是4环和3环.PAHs组成分析表明,几乎全部样品中PAHs均以高环(4~6环)为主,其高达60.5%~97.0%,仅在4个样品中检出了较高比例的低环PAHs (2~3环).这说明多数室内降尘中PAHs污染由交通运输(汽车和船舶)以及化工厂等高温燃烧排放造成.而安庆、芜湖及六安地区可能存在较严重的石油污染或煤、木材等低温燃烧源污染.公共场所、城市家庭和农村家庭降尘中PAHs的浓度存在明显的差异,总体上呈现:公共场所>城市家庭>农村家庭.异构体分析表明,公共场所和城市家庭内存在混合来源,而农村家庭以燃烧源为主.致癌能力分析表明,城市家庭降尘中的苯并[a]芘当量(BaPE)值略高于农村家庭.公共场所降尘中的BaPE值远大于家庭场所,是农村家庭或城市家庭场所的2倍多.     

Characterization and distribution of polycyclic aromatic hydrocarbon in sediments of Haihe River, Tianjin, China

In this study sediment samples were collected from 13 sites of Haihe River in Tianjin City, China, sixteen of priority polycyclic aromatic hydrocarbons （PAHs） listed in USEPA were analyzed by means of GC-MS. The total concentrations of PAH ranged from 774.81 to 255371.91 ng/g dw, and two to four rings of PAHs were dominant in sediment samples. Molecular ratios, such as phenanthrene/anthracene, fluoranthene/pyrene and low-molecular-weight PAH/high-molecular-weight PAH, were used to study the possible sources of pollution. It indicated a mixed pattern of parolytic and petrogenic inputs of PAHs in sediments in Haihe River. The petrogenic PAHs may be mainly derived from the leakage of refined products, e.g., gasoline, diesel fuel and fuel oil vehicle traffics or gas stations from urban area. The pyrolytic PAHs might be from the discharge of industrial wastewater and the emission of atmospheric particles from petrochemical factories. In addition, the levels of PAHs in the urban and industrial areas are far beyond the values reported from other rivers and marine systems reported. This situation may be due to polluted discharging from some petrochemical industrial manufactories and worse traffic conditions in Tianjin.     

城区叶面尘特性及其多环芳烃含量

用多步连续洗脱方法采集了干线道路路侧和远离道路校园内冬青卫矛叶面积尘,研究了叶面尘的采集方法.测定了2类叶面尘的粒径分布、有机碳含量和多环芳烃含量.结果表明,所测样品上的叶面尘可以在超声条件下4min一步洗脱.路边样品叶面尘积累量几乎是校园样品的2倍.2样品粒径分布基本形态非常相似,包括200μm以上和以下2个组分.后者占绝对优势.但校园内样品叶面尘粒径明显小于路边样品,两者粒径中位数分别为17.2μm和23.1μm.路边样中相对较粗部分显然来自机动车行驶扰动.由于颗粒较细,采自校园叶面尘中多环芳烃含量略高于路边样品.但不同多环芳烃分布谱非常相似.     

不同粒径地表街尘中重金属在径流冲刷中的迁移转化

在我国快速城市化进程中,街尘及其径流冲刷引起的重金属污染日显突出.通过对北京市城乡道路街尘及其人工降雨模拟径流冲刷过程中不同粒径街尘中重金属的分析,探讨街尘与径流冲刷过程中的粒径效应及不同重金属赋存形态的动态变化规律.结果表明,同一粒径颗粒物从"静态"街尘到"动态"径流中的颗粒物,重金属浓度呈下降趋势.街尘中重金属在径流冲刷过程中,存在溶解与解析现象,颗粒物粒径越小,减少比率越大,5种重金属(Cr、Cu、Ni、Pb、Zn)的减少比率分别为24.3%、56.8%、34.3%、22.8%、27.3%.街尘中的弱酸可提取态比例要略大于径流颗粒物中弱酸可提取态比例,部分以水溶态进入水体中.在径流冲刷过程中,水相溶解态重金属变化不大,水相颗粒态重金属含量随降雨时间径流过程迅速降低.固相颗粒物的重金属浓度随降雨时间总体上呈下降趋势.粒径越小,冲刷率越大,最大为62.1%,最小为4.6%.地表街尘在径流冲刷过程中,小粒径颗粒物具有较强的迁移能力,较容易进入水体造成污染.     

Influence of rice straw burning on the levels of polycyclic aromatic hydrocarbons in agricultural county of Taiwan

Atmospheric particulate and polycyclic aromatic hydrocarbons (PAHs) size distribution were measured at Jhu-Shan (a rural site) and Sin-Gang (a town site) in central Taiwan during the rice straw burning and non-burning periods. The concentrations of total PAHs accounting for a roughly 58% (34%) increment in the concentrations of total PAHs due to rice-straw burning. Combustion-related PAHs during burning periods were 1.54–2.57 times higher than those during non-burning periods. The mass median diameter (MMD) of 0.88–1.21 m in the particulate phase suggested that rice-straw burning generated the increase in coarse particle number. Chemical mass balance (CMB) receptor model analyses showed that the primary pollution sources at the two sites were similar. However, ricestraw burning emission was specifically identified as a significant source of PAH during burning periods at the two sites. Open burning of rice straws was estimated to contribute approximately 6.3%–24.6% to total atmospheric PAHs at the two sites.     

Polycyclic aromatic hydrocarbon in rain and street runoff in Amman, Jordan

Concentrations of polycyclic aromatic hydrocarbons(PAHs) were determined in the rain and street runoff samples from two sites in the vicinity of Amman City during the pluvial period 1999--2000. The results showed that elevated levels of PAHs were detected in the city center(site 1 ) than the residential area( site 2) and that the levels were higher in street runoff than rain samples of the same sites. The highest concentration of PAHs in both street runoff and rain samples were observed in the first rainy month( November 1999) which indicated a wash out effect of PAHs originating from vehicular emission accumulated during the long dry summer season before sampling. Within the investigated cold winter seasons, fluctuations in PAHs concentration were observed. The variation was attributed to the fossil combustion for heating purposes and to intervals between rainfalls: as the longer the intervals between rains were, the higher the PAH concentration were. Removal of PAHs from the atmosphere through precipitation over the investigated period varied with time and places depending on the amount of rainfall where higher rainfall removed higher amount of PAHs from the almosphere. The amount of PAHs washed out through precipitation was estimated to be around 14.8 mg/m^2 and 21.1 mg/m^2 for sites 1 and 2 respectively.     

城市灰尘PAHs累积与迁移过程的影响因素研究

以上海市为例,探讨了城市中心城区地表灰尘中多环芳烃(PAHs)累积与迁移过程的影响因素.结果表明,粒度只是影响城市灰尘吸附PAHs的一个次要因子,与PAHs含量之间没有明显的相关关系.城市灰尘TOC与PAHs含量显著正相关(冬季r=0.62,p＜0.000 1;夏季r=0.55,p=0.002),说明对于城市地表灰尘而言,有机质的含量越高,其吸收PAHs的能力就越强,这种结果与理论上PAHs的憎水亲脂性相一致.风向能够直接影响PAHs在空间上的分布趋势,污染源下风向的地区更容易累积较多的PAHs,且距离污染源越近,污染程度越重,相反,污染源上风向的地区则不利于PAHs的累积,污染程度较轻.夏季最高值出现在西北城区,含量为27 766 ng·g-1,冬季最高值出现在南部和东部城区,含量分别为30 741 ng·g-1和32 573 ng·g-1.大城市中心区存在PAHs污染的"空心效应".温度是影响城市灰尘PAHs累积与迁移的重要气象参数.     

重庆市主城区排水管道沉积物性质研究

为了解重庆市主城区排水管道沉积物的性质,调研和采集了生活区、交通区、文教区、商业广场等不同功能区的排水管道沉积物,分析了沉积物的粒径、密度、有机物含量(VSS/TSS)和污染物含量等指标,研究了不同功能区沉积物的差异.结果表明:不同功能区排水管道沉积有不同的理化性质,沉积物的粒径,交通区>文教区>商业广场>居住区.沉积物的密度与有机物含量(VSS/TSS)呈负相关(R2=0.998).沉积物污染物含量空间分异性显著,COD含量,文教区>居住区>商业广场>交通区.TN和TP含量,文教区>商业广场>居住区>交通区,与街尘相比,TP呈现显著富集特点.对于重金属含量,交通区显著高于其他3个功能区,Cu、Zn、Pb、Cd 最大值分别为303.5、539、104、1.14mg/kg.     

天津市城市扬尘及土壤尘单颗粒质谱特征

为探究城市扬尘及不同类型的土壤尘单颗粒质谱特征,使用SPAMS（单颗粒气溶胶质谱仪）对天津城市扬尘及不同类型土壤尘（菜地、果园、林地、农田）进行分析.结果表明:天津城市扬尘粒径在0.5~1.0 μm之间的占比较高;4种土壤尘在不同粒径段的分布略有差异,整体而言小粒径段（0.2~1.0 μm）占比低于大粒径段（1.0~2.0 μm）,说明土壤尘更易分布在大粒径段.在小粒径段,天津城市扬尘颗粒含有更多的碳组分及硫酸盐,大粒径段含有较多的金属、氯、硝酸盐、磷酸盐及硅酸盐组分.与城市扬尘相比,土壤尘中23Na+、46NO₂-峰强显著降低,39K+、35Cl-、42CNO-峰强增高,通过其峰强比值分布可将城市扬尘与土壤尘明显区分.与城市扬尘相比,土壤尘中含碳颗粒显著减少,同时出现钾类颗粒.城市扬尘作为一种混合源,含碳颗粒可能受多种排放源（机动车、燃煤等）影响,而土壤尘中钾类颗粒可能与农作物施肥有关.两种源类含27Al+、26CN-、35Cl-、42CNO-、46NO₂-、76SiO₃-、79PO₃-的颗粒占比均高于50%,其中40Ca+、46NO₂-和62NO₃-颗粒在天津城市扬尘中占比更高,76SiO₃-颗粒在土壤尘中占比更高,表明天津城市扬尘中更多的颗粒含有钙和硝酸盐组分,土壤尘中含硅酸盐颗粒较多.与机动车尾气、生物质燃烧等排放的颗粒物相比,天津城市扬尘及土壤尘中含97HSO₄-颗粒占比较低,表明天津城市扬尘及土壤尘颗粒中含有更少的硫酸盐,可作为将天津城市扬尘、土壤尘与其他源类区分的指标.      

广州秋季不同功能区大气颗粒物中PAHs粒径分布

利用MOUDI^TM级联分段式采样器采集了秋季广州市区(荔湾采样点和五山采样点)及郊区(新垦采样点)3个采样点的气溶胶样品并使用GC-MS分析了样品中13种多环芳烃的含量.发现3～4环的多环芳烃呈双峰分布,5～7环的多环芳烃呈单峰分布.广州市区和郊区的多环芳烃具有不同粒径分布模式;相对于城区,郊区的多环芳烃存在于更大的颗粒物中,这可能是气溶胶的陈化过程不同导致的.城区的多环芳烃可能主要受吸附作用控制,而郊区的多环芳烃则可能受多种机制控制,如吸附作用、吸收作用和多层吸附.诊断参数值在粒径1～2.5μm和0.1～0.56μm存在较大差异;从浓度上看新垦13种多环芳烃的总浓度为39ng/m³,五山为71～94ng/m³,荔湾为32～154 ng/m³;从组成上看广州市大气颗粒物种多环芳烃以5～7环为主.     

东海表层沉积物中多环芳烃的分布特征及来源解析

本研究对东海沉积物中多环芳烃(PAHs)组成及含量进行了分析,发现多环芳烃总浓度为8.2~180.2 ng/g,和国内外其它区域相比,整体处于一个低至中等程度的污染水平。东海沉积物中PAHs的分布整体表现为中间低、两端高的格局。内陆架是长江入海物质的主要沉积区,也是PAHs的主要汇集区;陆架北部区域的物质来源复杂,但总体受长江入海泥沙的控制,自西向东PAHs含量梯度递减;研究区域的东北部,较高的PAHs可能源于济州岛的输入;冲绳海槽也含有较高PAHs;而残留沉积区中PAHs含量极低。通过多环芳烃组成特征判断,东海表层沉积物中PAHs主要来自煤、木材、油类的燃烧,还有部分来自油类的泄漏。同时不同区域Ba P/Be P、Ba A/Chry比值的差别表明内陆架及冲绳海槽的PAHs主要来自河流输送,残留沉积区的PAHs可能主要来自大气沉降。     

Sedimentary record of polycyclic aromatic hydrocarbons in Lake Erhai, Southwest China

The temporal distribution of polycyclic aromatic hydrocarbons (PAHs) was investigated in a sediment core from Lake Erhal in Southwest China using gas-chromatography/mass spectrometry (GC/MS) method.The total organic carbon (TOC) normalized total PAHs concentrations (sum of US Environmental Protection Agency proposed 16 priority PAHs) ranged from 31.9 to 269 μg/g dry weight (dw),and were characterized by a slowly increasing stage in the deeper sediments and a sharp increasing stage in the upper sediments.The PAHs in the sediments were dominated by low molecular weight (LMW) PAHs,suggesting that the primary source of PAHs was low- and moderate temperature combustion processes.However,both the significant increase in high molecular weight (HMW) PAHs in the upper sediments and the vertical profile of diagnostic ratios pointed out a change in the sources of PAHs from low-temperature combustion to high-temperature combustion.The ecotoxicological assessment based on consensus-based sediment quality guidelines implied that potential adverse biological impacts were possible for benzo(ghi)perylenelene and most LMW PAHs.In addition,the total BaP equivalent quotient of seven carcinogenic polycyclic aromatic hydrocarbons (BaA,CHr,BbF,BkF,BaP,DBA and INP) was 106.1 ng/g,according to the toxic equivalency factors.Although there was no great biological impact associated with the HMW PAlls,great attention should be paid to these PAH components based on their rapid increase in the upper sediments.     

太湖表层沉积物中PAHs和PCBs的分布及风险评价

采用GC-EI-MS联用技术分析了太湖18个表层沉积物样品中多环芳烃(PAHs)和多氯联苯(PCBs)的含量.共检出28种PAHs,其总浓度范围为90.6~1.04×103ng/g,其中16种优控PAHs的浓度范围为63.1~885ng/g,最高浓度出现在竺山湖;56种PCBs的浓度范围为1.35~13.8ng/g,最高浓度出现在新塘港.利用分子比和因子分析/多元线性回归模型分析PAHs的来源,结果显示,太湖PAHs主要来源于燃烧,其中木柴、煤炭燃烧和油料燃烧的贡献率分别为45%和50%.PCBs同族体组成分析结果表明,PCBs的同系物组成呈现Aroclor 1242和Aroclor 1254的混合来源特征.太湖表层沉积物中PAHs和PCBs的二 毒性当量(以TCDD计)范围为0.64~3.35pg/g,风险评价结果表明,太湖沉积物中的PAHs和PCBs尚未对周围环境造成不利影响.     

宿州市街尘重金属的粒径分布特征及污染评价

在宿州市不同功能区采集23个街尘样品,利用X-Ray荧光光谱法测定了样品中重金属Cu、Zn、Pb、Mn、Cr、V的含量,分析了街尘重金属的粒径分布特征,并利用地累积指数法对其污染状况进行了评价。结果表明:(1)宿州市街尘中细颗粒质量比重较高,在<75μm、75～150μm、150～250μm、250～500μm四个粒径段的街尘质量比例分别为39.73%、27.52%、22.57%和10.18%;(2)街尘中各重金属元素的含量最大值均出现在<75μm和75～150μm粒径范围内,说明重金属易在细颗粒中富集;(3)各重金属元素在<75μm粒径范围内的赋存比例均高于其他3个粒径级别,达40%左右;(4)随着街尘粒径的由粗到细,其重金属污染程度从无污染到轻度污染,各重金属元素的污染程度依次为:Zn>Pb>Cr>Cu>V>Mn。     

白洋淀表层沉积物中多环芳烃的含量、分布、来源及生态风险评价

研究了白洋淀表层沉积物中US EPA 16种优先控制的多环芳烃(PAHs)的分布特征和污染来源,其w(PAHs)为101.3～1 494.8 ng/g (平均值为353.0 ng/g),与国内其他的湖泊和河流相比,整体处于中等污染水平. 安州采样点沉积物中w(PAHs)最高,污染最严重;其次为小田庄、烧车淀、王家寨;污染较轻的采样点为枣林庄、光淀、圈头和端村. 在16种多环芳烃单体中,菲、荧蒽、芘、苯并［b］荧蒽所占比例较大. w(荧蒽)/w(芘)和w(菲)/w(蒽)2个比值显示, 白洋淀沉积物中多环芳烃的含量和分布受石化材料燃料、煤炭及薪柴燃烧影响较大. 风险评价表明,安州采样点表层沉积物对生物存在潜在危害,而其他采样点沉积物潜在风险处于较低水平.      

福州市区街道灰尘中多环芳烃的质量分数及其来源

采用超高效液相色谱系统(UPLC)荧光检测器法,测定了福州市区14条主要街道灰尘样品中属美国环境保护署(US EPA)优控的15种多环芳烃(PAHs)的质量分数,对其毒性进行了评估,并通过聚类分析、因子分析/多元线性回归等方法,分析了灰尘中PAHs的来源. 结果表明:福州市区的w(PAHs)为1 029.5～5 182.0 μg/kg,平均值为2 884.7 μg/kg,在国内外城市中处于中等含量水平. 14个街道灰尘样品中有5个样品的w(PAHs)超过毒性效应区间低值(ERL),具有潜在的生态风险. 聚类分析发现,4号,5号,7号和12号采样点分别具有高比例的w(菲),w(苯并［b］荧蒽),w(荧蒽)和w(萘)的特殊来源.对样品中PAHs的来源解析显示,燃烧源占78%,石油泄漏源占22%.      

北运河流域(北京段)沉积物中PAHs污染特征与风险评估

为探明北运河流域（北京段）多层沉积物中PAHs（多环芳烃）的污染状况,利用活塞式底泥取样器于2014年11月采集了9处沉积物样品,取样深度为30~80 cm,每处样品根据其垂向介质特征大致分成3~4层,分别测定各层样品的粒径、TOM（总有机质）及16种PAHs的质量分数,探讨PAHs在河道沿程与垂向上的分布特征、来源及生态风险评价.结果表明,北运河流域（北京段）沉积物以砂质壤土为主,w（TOM）（以干质量计,下同）为103.4~146.8 g/kg,w（∑₁₆PAHs）为598.1~28 730.6 ng/g,各层w（∑₁₆PAHs）为108.5~8 810.8 ng/g.沉积物中PAHs以高环为主,主要包括有Phe（Phenanthrene,菲）、Fla（Fluoranthene,荧蒽）、Pyr（Pyrene,芘）、BbF〔Benzo（b）fluoranthene,苯并[b]荧蒽〕.在河道沿程变化上,中下游沉积物的污染程度远高于上游.在垂向变化上,w（TOM）和沉积物粒径对PAHs的分布影响有限,PAHs的垂向分布主要受所处沉积环境与历史污染程度影响.根据主成分分析与同分异构体比值法推断,PAHs主要来源于化石燃料与生物燃料的燃烧,少部分为石油源.利用效应区间值得出的生态风险评价结果表明,北运河流域（北京段）沉积物中PAHs可能已对环境产生负面影响,其中BbF、BkF、InP与BgP已对环境产生毒副作用,需要给予关注与解决.      

Size distribution of particulate polycyclic aromatic hydrocarbons in fresh combustion smoke and ambient air: A review

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous in the atmosphere and they mostly stem from the imperfect combustion of fossil fuels and biofuels. PAHs are inherently associated with homogenous fine particles or distributed to different-sized particles during the aging of air masses. PAHs carried by fine particles undergo a long-range transport to remote areas while those adsorbed on coarse particles have a shorter lifetime in ambient air. More importantly, PAHs with higher molecular weights tend to be bound with finer particles and can deeply enter the lungs, posing severe health risks to humans. Thus, the environmental fate and health effects of particulate PAHs are strongly size-dependent. This review summarizes the size distributions of particulate PAHs freshly emitted from combustion sources as well as the distribution patterns of PAHs in ambient particles. It was found that PAHs from stationary sources are primarily bound to fine particles, which are slightly larger than particles to which PAHs from mobile sources are bound. In ambient air, particulate PAHs are distributed in larger size modes than those in the combustion fume, and the particle size decreases with PAH molecular weight increasing. The relevant mechanisms and influencing factors of particle size distribution changes are illustrated in this article, which are essentially attributed to combustion and ambient temperature as well as the physical and chemical properties of PAHs. Overall, the study on the particle size distribution of PAHs will contribute for a full understanding of the origin, atmospheric behaviors and health effects of particulate PAHs.