Polycyclic aromatic hydrocarbons (PAHs) in a sediment core from Lake Taihu and their associations with sedimentary organic matter

Sediment core is the recorder of polycyclic aromatic hydrocarbon (PAH) pollutions and the associated sedimentary organic matter (SOM), acting as crucial supports for pollution control and environmental management. Here, the sedimentary records of PAHs and SOM in the past century in Lake Taihu, China, were reconstructed from a 50-cm sediment core. On the one hand, the presence of PAHs ranged from 8.99 to 199.2 ng/g. Vertically, PAHs declined with the depth increased, and the sedimentation history of PAHs was divided into two stages with a discontinuity at 20 cm depth. In composition, PAHs in the sediment core were dominated by three-ring PAHs (44.6% ± 9.1%, mean ± standard deviation), and were followed by four-ring (27.0% ± 3.3%), and five-ring (12.1% ± 4.0%) PAHs. In toxicity assessment, the sedimentary records of benzo[a]pyrene-based toxic equivalency were well described by an exponential model with R-square of 0.95, and the environmental background toxic value was identified as 1.62 ng/g. On the other hand, different components of SOM were successfully identified by n-alkane markers (p < 0.01) and the variations of SOM were well explained (84.6%). A discontinuity of SOM was recognized at 22 cm depth. Association study showed that the sedimentary PAHs were associated with both anthropogenic and biogenic SOM (p < 0.05) with explained variances for most individual PAHs of 60%. It indicated the vertical distributions of PAHs were driven by sedimentary SOM. Therefore, environmental processes such as biogenic factors should attract more attentions as well as PAH emissions to reduce the impacts of PAHs.     

官厅水库周边蔬菜地表土中多环芳烃的污染

为掌握北京市备用水源地——官厅水库周边的蔬菜地表土中多环芳烃(PAHs)的污染状况及来源,于2008年11月在延庆县小丰营蔬菜产地采集了48个表土样品(0～20cm)测定PAHs含量,并综合特征化合物比值法和因子分析/多元线性回归两种方法推断了土壤中PAHs来源.结果表明,土壤中15种PAHs单体(PAH15)的含量均服从正态分布或对数正态分布,∑15PAH几何均值为(118.71±28.63)ng.g-1(干重含量,下同),算术均值为(139.57±85.65)ng.g-1.以荷兰土壤标准衡量,71%的样点归类PAHs弱污染,与文献报道的大多数国内外农业土壤相比,尚属于较清洁的水平.成分谱分析表明,研究区域土壤中的PAHs分布谱以3环～4环化合物为主,优势化合物为PHE、FLA、FLO、PYR.校正后的FLA/(FLA+PYR),ANT/(ANT+PHE)比值表明该研究区域PAHs主要来自燃烧源.通过因子分析提取了3个主成分,分别代表①燃煤和交通燃油;②生物质燃烧和炼焦;③燃油.多元线性回归分析的结果表明,这3种来源对官厅水库周边蔬菜地表土中PAHs的贡献分别是54.0%,39.9%和6.1%.结合两种源解析方法和排放源分析,除该区域存在明显生物质燃烧源以外,其它来源的PAHs经过了一定距离的大气迁移和沉降.     

长江和辽河沉积物中的多环芳烃类污染物

报道了长江和辽河沉积物中17种多环芳烃（PAHs）类污染物的含量及分布状况．所研究的长江南京段沉积物中多环芳烃总量变化范围为213.8～550.31ng/g（干重）,辽河新民段沉积物中多环芳烃总量变化范围为 27.45～198.26ng/g（干重）．测定结果表明,长江和辽河沉积物中多环芳烃具有不同的空间分布模式：长江段以南京市下游的沉积物中PAHs含量为最高,而辽河段则以新民市区的沉积物中PAHs含量为最高但总的来说,长江南京段沉积物中多环芳烃的污染水平明显高于辽河新民段沉积物所受的多环芳烃污染．     

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.     

Biodegradation of polycyclic aromatic hydrocarbons (PAHs) by fungal enzymes: A review

Polycyclic aromatic hydrocarbons (PAHs) are a large group of chemicals. They represent an important concern due to their widespread distribution in the environment, their resistance to biodegradation, their potential to bioaccumulate and their harmful effects. Several pilot treatments have been implemented to prevent economic consequences and deterioration of soil and water quality. As a promising option, fungal enzymes are regarded as a powerful choice for degradation of PAHs. Phanerochaete chrysosporium, Pleurotus ostreatus and Bjerkandera adusta are most commonly used for the degradation of such compounds due to their production of ligninolytic enzymes such as lignin peroxidase, manganese peroxidase and laccase. The rate of biodegradation depends on many culture conditions, such as temperature, oxygen, accessibility of nutrients and agitated or shallow culture. Moreover, the addition of biosurfactants can strongly modify the enzyme activity. The removal of PAHs is dependent on the ionization potential. The study of the kinetics is not completely comprehended, and it becomes morem hallenging when fungi are applied for bioremediation. Degradation studies in soil are much more complicated than liquid cultures because of the heterogeneity of soil, thus, many factors should be considered when studying soil bioremediation, such as desorption and bioavailability of PAHs. Different degradation pathways can be suggested. The peroxidases are heme-containing enzymes having common catalytic cycles. One molecule of hydrogen peroxide oxidizes the resting enzyme withdrawing two electrons. Subsequently, the peroxidase is reduced back in two steps of one electron oxidation. Laccases are copper-containing oxidases. They reduce molecular oxygen to water and oxidize phenolic compounds.     

太湖多环芳烃的历史沉积记录

通过分析测定太湖上、下2个典型湖湾(梅梁湾和东山胥口湾)沉积钻孔中多环芳烃的垂直分布和含量特征,结合210Pb定年,重建了该地区多环芳烃的历史沉积记录.研究发现,梅梁湾沉积物PAHs污染年代早并重于胥口湾,但两地PAHs污染类型基本相似.在剖面深度0～28cm范围内,梅梁湾和胥口湾多环芳烃的沉积通量范围分别为40～320ng·cm-2·a-1和13～150 ng·cm-2 a-1.自上世纪40年代起,梅梁湾沉积物中的PAHs通量呈不断上升之势,近25年来增加更为迅速,可能源于太湖北部湖区乡镇工业的快速发展;而胥口湾的PAHs污染只在1990年之后才开始加重,并呈急剧增加之势态.太湖沉积物中的多环芳烃主要为热(燃烧)成因来源,沉积物中高环PAHs的比例呈递增趋势,流域内能源消耗和机动车尾气排放的增加是其主导因素.多环芳烃的沉积记录很好的反映了周边地区社会经济的发展变化,反映了人类活动与水环境污染状况之间的关系,提示经济发展过程中环境保护的相对滞后.     

滇池PAHs的沉积记录、来源及其生态风险评估

采用GC/MS方法分析了滇池沉积柱中16种美国EPA优控的多环芳烃(PAHs)的垂直分布状况,并对其来源变化及生态风险进行了分析和评估.研究表明:滇池沉积柱中PAHs的含量范围为558～6418 ng·g-1,并在20世纪90年代初达到峰值,这明显不同于发达国家的同类研究,也与国内沿海地区和偏远湖泊的相关研究有所不同.滇池沉积物中的PAHs主要来自当地的家庭燃煤、木材和生物秸秆等的低温燃烧过程,但工业燃煤和机动车尾气等高温燃烧过程释放的PAHs的相对含量近年来有明显增加的趋势.风险评估结果显示,滇池中上层沉积物中的PAHs可能存在潜在的生态风险,而这些生态风险主要来自低环数的NAP、FLU、PHEN和高环数的BbF、BaP、DBA等.     

多环芳烃(PAHs)在大气中的相分布

通过对广州市老城区空气中多环芳烃的研究表明 ,该区多环芳烃的污染相当严重 ,不同季节测定的多环芳烃总量差别不大 ,但颗粒相多环芳烃在春季占的比例 (44 8% )要高于夏季 (9 4 % ) .气相中主要以芴、菲、甲基菲、荧蒽、芘等低环数的多环芳烃为主 ,而高于四环的多环芳烃主要是分布在颗粒相中 ,苯并 (ghi)是最主要的颗粒相多环芳烃物质 .     

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%.     

基于原位被动采样技术研究巢湖沉积物和水体中PAHs的垂直分布及其界面交换

沉积物-水体界面处分子扩散是污染物的一个重要地球化学过程,也是判断沉积物是否为上层水体中污染物汇或源的主要依据.本研究利用低密度聚乙烯膜(LDPE)为吸附相的原位被动采样器,同步确定了巢湖西半湖南淝河入湖口处不同深度的上层水体和沉积物孔隙水中13种多环芳烃(PAHs)浓度,并计算了它们在沉积物-水体界面的分子扩散通量.结果表明,3种性能参考化合物(PRCs)在上层水体中的解析速率较沉积物孔隙水中大,相应地,水体中LDPE膜对PAHs的吸附速率高于沉积物孔隙水.水体中13种PAHs总浓度(130～250 ng·L~(-1))低于沉积物孔隙水(180～253 ng·L~(-1)),且均以低环PAHs为主.2～3环PAHs浓度在上层水体中无明显的垂直变化,但4～6环PAHs浓度呈现随深度增加而降低的趋势.沉积物孔隙水中PAHs浓度的垂直变化规律反映了历史强排放过程.研究区域PAHs在沉积物-水体界面的交换通量变化范围为-384～1445 ng·m~(-2)·d~(-1),除Flu和Pyr外,其它PAHs均从沉积物向水体释放,反映了底部沉积物是上层水体中PAHs的重要二次污染源.     

我国腾冲大气PAHs的可能来源分析

2005年10月22日至2006年10月21日,在云南腾冲一典型背景点进行了每周一次的大气采样,以监测季风期东南亚地区生物质燃烧导致的多环芳烃(PAHs)的输入状况.结果表明,监测期内总PAHs含量为43.1~156ng/m3 (平均值为87.9ng/m3).其中气相PAHs均值为85.8ng/m3,无明显的季节变化;颗粒相PAHs均值为2.35ng/m3,在春季出现显著高值,可能与东南亚生物质燃烧释放的PAHs在南亚季风作用下向腾冲的跨境迁移有关.颗粒相PAHs以毒害性较大的高环PAHs化合物为主,其在偏远地区生态系统中的累积可能带来一定的生态风险.     

Source apportionment of polycyclic aromatic hydrocarbons (PAHs) in a sediment core from Lake Dagze Co, Tibetan Plateau, China: Comparison of three receptor models

Receptor models are a useful tool for identifying sources of polycyclic aromatic hydrocarbons (PAHs) in multiple environmental media. In this study, three different receptor models (including the principal component analysis-multiple linear regression (PCA-MLR), positive matrix factorization (PMF), and Unmix models) were used to apportion the sources of 16 priority PAHs in a sediment core of Lake Dagze Co. The ∑PAHs (sum of all 16 measured PAHs) concentrations ranged from 51.89 to 132.82 ng/g with an average of 80.39 ng/g. The ∑PAHs were dominated by 2-3 ring PAHs, accounting for 80.12% on average, thereby indicating that they mainly originated from biomass and coal combustion and/or from long-range atmospheric transportation. The three models produced consistent source apportionment results. The greatest contributor to ∑PAHs was biomass combustion, followed by coal combustion, vehicle emissions, and petrogenic sources. Moreover, the temporal variation of the common sources was well-correlated among models. The multi-method comparison and evaluation results showed that all three models were useful tools for source apportionment of PAHs, with the PMF model providing better results than the PCA-MLR and Unmix models. The temporal trends of factor contributions were verified by PAHs with different ring numbers. Significant correlations were found between the simulated concentrations of each source factor and the PAHs with different ring numbers (P<0.01), except for the petrogenic source identified by the Unmix model (P>0.05). This study can provide useful information for further investigation of source apportionment of PAHs in the sediment cores.     

渤海湾潮滩不同粒径沉积物中多环芳烃的分布

利用湿筛分离的方法,将采自渤海湾潮间带的沉积物分成0.063mm 3个不同的粒径组分,测定其16种EPA规定的多环芳烃(PAHs)含量、总有机碳(TOC)和碳黑(BC)含量.结果表明,不同粒径沉积物中∑PAHs含量范围在714~4870ng/g之间.在岐口(TS3)沉积物中,∑PAHs含量最高值出现在0.063mm粒径组分中.所有站点沉积物的0.031~0.063mm粒径组分中∑PAHs含量均为最低.尽管如此,有机碳标准化∑PAHs含量则随着沉积物粒径的增大呈现增加趋势.不同粒径沉积物中∑PAHs含量与BC含量之间呈现显著正相关关系,而与有机碳(OC=TOC-BC)含量之间的相关性较差.因此,不同粒径沉积物中BC的分布很可能在其中扮演着更重要的作用.     

我国一些城市污泥中多环芳烃(PAHs)的研究

应用GC／MS对我国内地和香港地区共11个城市污泥中的17种多环芳烃化合物（PAHs）进行了研究，各城市污泥中∑PAHs的含量在2．271－143．804mg/lg之间，依次为兰州污泥＞珠海污泥＞北京污泥＞广州污泥＞佛山污泥＞无锡污泥＞沙田污泥（香港）＞元朗污泥（香港）＞大埔污泥（香港）＞西安污染＞深圳污泥，含量较高的化合物主要是蒽、荧蒽、苯并（a）蒽和屈等，珠海污泥和北京污泥的苯并(a）芘含量超过我国城市污泥农用标准，各化合物的最高含量分别分布在兰州污泥、珠海污泥、北京污泥和广州污泥中，各城市污泥中的PAHs具有不同的分布特征，均以少数化合物为主，主要是3和4个苯环的化合物，2、5和6个苯环的化合物含量普遍较低。     

滴水湖水系沉积物中多环芳烃的分布及风险评价

2012年,每两个月采集一次上海人工滩涂湖泊——滴水湖水系表层沉积物,检测16种多环芳烃(PAHs)含量.结果表明,滴水湖水系∑PAHs变化范围为74.03~579.20ng/g,平均值为272.55ng/g.其中,闸外引水河[(407.64±6.90)ng/g]≈闸内引水河[(427.99±213.84)ng/g]>滴水湖[(156.33±62.00)ng/g].研究区各点蒽/(蒽+菲)比值均大于0.1,说明PAHs主要来自于石油燃烧源.生态风险评价表明,滴水湖水系沉积物PAHs不存在严重的生态风险,但闸外和闸内引水河沉积物PAHs存在较低几率的潜在风险,湖区沉积物PAHs则无潜在风险.     

珠江口现代沉积物柱芯样多环芳烃高分辨沉积记录研究

通过对采集于珠江三角洲澳门河口区的沉积物柱状样品中多环芳烃的GC MS定量分析测定,并结合210Pb同位素定年分析,重建了珠江口近代有机污染物的污染史(1959～1996年).研究结果表明,柱芯样品中多环芳烃的浓度为0.6～4.5μg·g-1(干重计),污染程度为中等.其中在20世纪60年代和80年代分别记录到两个高的污染峰,表明这两个时间段内有较大的污染物输入.以母体化合物比值对沉积物样品中的多环芳烃来源进行了分析,结果表明是受到了以油类和不完全燃烧产物为主的混合污染,且污染来源较为单一.对沉积物毒性潜在效应的计算表明,表层沉积物毒性效应较大,且从90年代初期开始后至1996年,毒性当量浓度呈线性趋势增加.     

几种多环芳烃的植物吸收作用及其对根系分泌物的影响

采用水培试验方法,以多年生黑麦草(Lolium multiflorum Lam.)为供试植物,研究了芘、菲、苊和萘的植物吸收作用及其对根系分泌物的影响.结果表明,黑麦草能明显吸收富集多环芳烃(PAHs);随培养液中PAHs浓度的升高,其在黑麦草根和茎叶中的含量增大,且根的PAHs含量、富集系数要远大于茎叶.芘、菲、苊、萘污染胁迫下,黑麦草根系分泌物中可溶性有机碳、草酸和可溶性总糖的含量均高于无污染对照.供试污染浓度范围内,随着培养液中菲、苊、萘浓度提高,可溶性有机碳、草酸及可溶性总糖的分泌量增大;但在芘胁迫下,与污染对照相比,分泌量的增加幅度随着芘浓度的升高则呈先增大后减小的趋势.在较低污染强度下,供试PAHs对根系分泌物的促分泌效应由强到弱依次为芘、菲、苊和萘.4种PAHs对可溶性糖类的促分泌作用最强,其分泌量的增加幅度明显大于可溶性有机碳和草酸.     

中国沉积物多环芳烃的时空分布及驱动因子

根据2000～2020年中国湖泊、河流和河口沉积物中多环芳烃(PAHs)的时空分布,并通过构建结构方程模型和重力模型分析了驱动PAHs时空分布的社会经济因素.结果表明,不同地区沉积物中PAHs含量由高到低依次为：北部沿海>东北>东部沿海>南部沿海>黄河中游>长江中游>西南>西北.南部沿海、长江中游和东部沿海地区高分子量PAHs的比例相对较高,东北、西北、北部沿海和黄河中游地区低环PAHs的比例相对较高.沉积物中PAHs的含量从2000年起逐渐增加,2006年以后逐渐减少,且不同地区沉积物中PAHs含量到达峰值的年份有显著差异.经济发达地区沉积物中PAHs的含量在达到峰值后逐渐下降;发展中地区由于经济发展较快导致污染物积累较快.偏远或欠发达地区PAHs含量逐渐增加,但累积率低于发达地区.城市化和工业化对沉积物中PAHs的影响显著,其中对沉积物中PAHs分布影响最大的因素为经济发展.     

深圳市大气中多环芳烃的污染特征与来源识别

利用大流量主动采样器于2009年12月~2010年1月及2010年6月,分冬季与夏季两批次对深圳市13个点位进行大气样品采集,检测其气相及颗粒相中总的多环芳烃(PAHs)浓度.结果表明,冬季深圳市大气中总PAHs的浓度为17.9~92.3ng/m3,平均值为45.3ng/m3;夏季总PAHs浓度范围为8.64~96.3ng/m3,平均值为32.2ng/m3.两个季节PAHs单体中均以3~4环为主,占总浓度的75%以上;单个组分与总量的相关性分析表明,夏季明显优于冬季.来源分析表明,冬季大气中PAHs来源比夏季更为复杂,通过特征分子比值法推断冬季PAHs主要来源于石油源、燃煤、机动车尾气排放;夏季主要来源于机动车尾气排放.利用毒性当量因子法和致癌风险评价其污染水平和毒性风险,结果表明深圳市大气中PAHs污染与国内部分城市相比,处于较低水平.     

深圳大运会期间大气中多环芳烃的特征及消减情况研究

深圳大运会期间,利用大流量主动采样器对深圳市5个点位进行大气样品采集,检测其气相及颗粒相中总的多环芳烃(PAHs)浓度以及与2010年夏季的监测数据进行比较,研究PAHs通过各种空气质量保障措施实施后的消减情况.结果表明,大运期间5个点位∑PAHs变化范围为15.80~62.09ng/m3,平均值30.77ng/m3,与2010年夏季相比,PAHs平均消减28%;大运期间PAHs单体中均以3~4环为主,平均占总浓度的88%;通过特征分子比值法推断大运期间机动车尾气排放是PAHs的主要来源,但是柴油车尾气排放和燃煤电厂废气排放的贡献比率增加;大运期间∑BaPeq比2010年夏季降低36%,BaP浓度以及∑BaPeq浓度都低于我国环境空气中对BaP的限值标准;呼吸致癌风险评价表明,大运期间为每百万人致癌3.8例,2010年夏季为每百万人致癌7.3例,致癌风险下降48%.