广州市室内尘土中多溴联苯醚的分布特点及来源

随机采集了广州市46个家庭和12个办公室内尘土样品,同时采集了17个室外尘土样品、2个电视机和2个电脑尘土样品并分析了室内尘土中多溴联苯醚(PBDEs)的含量、单体分布及来源.结果表明,家庭尘土中∑10PBDEs(BDE28,47,66,85,99,100,153,154,183,209之和)的含量为 564.3~9654ng/g,中值和均值分别为 2686,3407ng/g;办公室尘土中∑10PBDEs 的含量为 1737~4408ng/g,中值和均值分别为3133,3179ng/g.室内尘土中PBDEs的最主要单体为BDE209,分别占家庭尘土和办公室尘土∑10PBDEs的97.4%和99.0%.BDE47、99和183在室内尘土中含量也较高.大多数室内尘土中∑10PBDEs的含量高于室外,说明室内可能有重要的PBDEs释放源.室内尘土中PBDEs的主要工业品来源为十溴联苯醚,五溴联苯醚次之,八溴联苯醚较少.     

典型污水处理厂中多溴联苯醚的分布特征、迁移及负荷研究

本研究通过对典型污水处理厂各构筑物进行采样分析,研究多溴联苯醚在污水处理厂中的分布、迁移和转化.结果表明,在污水处理厂所有污泥样品中都有PBDEs检出,PBDEs浓度范围在4226.76~9204.14 ng·g-1之间.其中,BDE-209是主导同系物,所占平均比例为83.16%(范围为75.75%~89.48%).该污水处理厂的进水样品中溶解态PBDEs总浓度为183.11 ng·L-1,而出水样品中溶解态PBDEs浓度则降至7.07 ng·L-1,PBDEs的去除率达到96%以上.所有污水样品中BDE-209都是最主要的同系物,所占比例在75.75%~85.68%之间,BDE-99和BDE-47是仅次于BDE-209的另外2种主要同系物.通过对污水处理流程中PBDEs的溶解态和颗粒态分配系数的研究得出,溶解性颗粒物对疏水性有机物在整个污水处理流程中的迁移、转化有重要的影响.该污水厂的日均PBDEs负荷量为21311.2 mg·d-1,污水经初沉池和二沉池处理之后分别有58.07%和39.91%的PBDEs被去除,即一共有97.98%的PBDEs被去除了,最后在出水中只剩2.02%的PBDEs.该污水厂通过出水的日均排放PBDEs的量为430.8 mg,通过脱水污泥日均排放PBDEs的量高达20880.4 mg.土壤在污泥农用之后PBDEs浓度年增加量为25.4μg·kg-1,污泥农用需要百年以上才能达到欧盟的规定限值.     

家庭尘土中多溴联苯醚的含量及人体暴露水平初步研究

在广州和海口随机采集了52个家庭尘土样品,用GC/MS定量分析了样品中∑10PBDEs(BDE28,47,66,85,99,100,153,154,183,209之和)的含量、单体组成模式和可能的影响因素,并估算了成年人和婴幼儿通过尘土摄入对PBDEs的暴露水平.结果表明,所有样品中都检出PBDEs,∑10PBDEs的含量范围为544.2～9 654 ng/g,中位值和平均值分别为2 547 ng/g和3 096 ng/g,广州样品中∑10PBDEs含量明显高于海口样品.尘土中PBDEs含量与家用电器和含聚氨酯泡沫家具数量、电器使用时间没有显著相关性.家庭尘土中PBDEs的主要成分是BDE209,其平均含量高达3 021 ng/g,占∑10PBDEs含量的73.70%～99.74%,平均值为96.85%.BDE47、99和183是∑9PBDEs(BDE209除外)中含量最丰富的单体,其含量均值分别为24.48%、23.99%和21.66%,广州和海口样品的单体组成没有显著区别.成年人和婴幼儿通过尘土摄入对PBDEs的暴露水平分别为10.59～254.7 ng/d和140.1～509.3 ng/d,由于婴幼儿的尘土摄入量远大于成年人,其对PBDEs的暴露水平也明显偏高.尘土摄入是人体暴露于PBDEs的重要途径,对婴幼儿更是如此.     

多溴联苯醚在河套农灌区土壤和水体中的分布特征

PBDEs作为一类全球性的新兴持久性有机污染物,因其具有疏水性,土壤和沉积物对其有很强的固着能力,被认为很难进入地下水中。文章在河套平原典型的黄河农灌区采集地下水、地表水以及表层土壤样品,利用GC-μECD和GC-MS方法测定发现,地下水和地表水中均检测到PBDEs,且主要为BDE209,其在地下水中含量高达5.3μg/L,而地表水中仅为0.03μg/L,揭示PBDEs存在污染地下水的可能性。对土壤中PBDEs的分析发现,其优势同系物为BDE47、100、183和99,主要富集在地面以下0~5 cm和10~15 cm处,该范围普遍发现农用地膜(PBDEs≤5μg/g)的残留物。此外,研究区主要农作物(玉米、番茄、瓜类、小麦和葵花)中,广泛利用地膜的玉米种植土壤中PBDEs的含量最高,达77.13 ng/g。研究显示,降雨淋滤以及灌溉水入渗作用下,地膜中PBDEs的释放可能是研究区土壤以及地下水中PBDEs不可忽略的重要污染源。     

西安城区秋季大气中多溴联苯醚的污染特征及来源分析

为了评估西安大气中多溴联苯醚（PBDEs）的污染程度,2008年8～10月,利用大流量主动采样器采集了西安城区气态和颗粒态大气样品.分别利用GC-MS和GC/ECD对低溴PBDEs和BDE-209进行分析,12种PBDEs的总浓度（气相＋颗粒相）范围为37.43～620.30 pg/m3,平均值为216.28 pg/m...     

南海北部大气气相多溴联苯醚的含量及来源

通过"实验三号"开放航次在南海北部采集了32个大气样品,用气相色谱/质谱联用仪分析了样品中的多溴联苯醚(PBDEs)同系物,并对其含量、组成特征、空间分布及主要来源进行了研究.结果表明,南海北部大气中7种PBDEs总浓度为0.07～35.9 pg.m-3,四溴(BDE-47)和五溴(BDE-99和-100)化合物为主要组成,分别约占PBDEs总量的51.5%和36.9%,显示工业五溴联苯醚的使用是其主要来源;中国东南沿海和菲律宾附近PBDEs浓度较高,南海靠近越南中部海域大气PBDEs含量较低.后推气流轨迹分析指出:我国东南沿海,特别是珠江三角洲,以及我国台湾和菲律宾等地区陆源污染物的外溢是引起南海北部地区PBDEs浓度较高的主要原因.     

江苏经济高速发展城市香樟树皮中的多溴联苯醚

2009年7月在江苏省南部城市苏州,南通和无锡采集了40组香樟树皮样品,用加速溶剂萃取、气相色谱质谱法测定了样品中8种多溴联苯醚（PBDEs）.结果表明,所有样品中都检出了PBDEs,Σ8 PBDEs（BDE28、47、100、99、153、154、183、209）平均含量为835μg/kg脂重（112～7 460μg...     

大亚湾海域多溴联苯醚的生物累积特征

 于2003年9月在大亚湾海域采集生物(鱼、虾、蟹和乌贼)样品,分析其多溴联苯醚(PBDEs)的浓度和脂含量,以及同位素δ¹⁵N与δ¹³C的值.结果表明,鱼、虾、蟹和乌贼的PBDEs总平均含量分别为5.43±3.97,1.18±0.67,3.37±2.33,5.66ng/g脂重.肉食性的鱼类PBDEs的生物累积比植食性的鱼类相对较高.BDE47为最优势组分,占总PBDEs的30%,且在所有样品中均被检出.生物体中PBDEs的含量与脂含量和δ¹⁵N值均呈正相关,脂含量对生物体富集PBDEs的影响远比生物所处的营养级的影响大.     

溴代阻燃剂对生物脱氮除磷的影响

为探究新兴污染物溴代阻燃剂（BFR）对生物脱氮除磷（BNPR）的影响,以实际废水为探究对象,建立厌氧/好氧/缺氧序批式反应器,中温环境下研究了不同浓度多溴联苯醚（PBDEs）对BNPR的影响。结果表明:PBDEs对BNPR的影响具有浓度依赖性,低浓度PBDEs对BNPR及污泥特征影响不明显,而ρ（PBDEs）>0.1 mg/L时可显著抑制BNPR。当PBDEs浓度为2.0 mg/L时,活性污泥系统稳定运行时化学需氧量（COD）、氨氮及正磷酸盐（OP）的去除率分别为73.2%~75.6%、85.2%和72.1%~73.6%,显著低于空白组。此外,PBDEs的存在可降低污泥内总悬浮固体和挥发性悬浮固体,提高污泥体积指数及胞外聚合物含量。典型周期研究发现PBDEs可抑制硝化、反硝化、厌氧释磷及好氧吸磷过程。     

海河流域14条河流表层沉积物中多溴联苯醚的分布特征

海河流域是我国受人类活动扰动强度最大的地区,为了解多溴联苯醚（PBDEs）在该流域的污染现状与分布特征,通过采集14条主要河流的48个表层沉积物样品,采用高分辨的GC-MS/MS技术对干燥后的沉积物中27种PBDEs进行分析.结果发现沉积物中PBDEs的平均含量范围为0.06～2.10 ng·g^-1;其中徒骇河沉积物...     

基于毒理基因组学的PBDE-209和镉联合毒性效应研究

多污染物引发的联合毒性是环境污染物风险评价中的重要问题之一,然而此类研究相对不足.多溴联苯醚和重金属镉可在多种环境介质中共存,虽对其各自单独暴露所产生的毒性已有相对明确的认识,但对二者联合毒性效应及其分子机制的探索仍十分有限.生物信息学的发展为污染物的健康效应研究提供了一种新的思路.为此,本研究基于比较毒理基因组学数据库(CTD)分析了十溴联苯醚和镉在单独或共同暴露下所影响的基因和相关疾病,推测两种污染物对胎儿红系造血过程产生的潜在影响,并进一步整合外源红系细胞基因表达数据库中的基因芯片确证二者共同影响的基因集合.同时,通过对这些基因集合进行生物学过程和信号通路富集分析,筛选出潜在的靶基因JAK3和AKT2,并在无显著细胞毒性的暴露条件下,通过体外细胞实验验证了十溴联苯醚和镉对这两个靶基因表达的干扰.本研究结果可为预防多溴联苯醚和重金属的联合暴露风险提供一定的科学依据,同时,CTD数据库和外源特定疾病发生发展相关基因表达数据库联合使用,并结合传统毒理学研究手段的评价模式,可为污染物的共同暴露与特定疾病的相关性及分子机理的探索在研究思路和技术手段上提供参考.     

Occurrence, distribution, and potential influencing factors of sewage sludge components derived from nine full-scale wastewater treatment plants of Beijing, China

Millions of tons of waste activated sludge (WAS) produced from biological wastewater treatment processes cause severe adverse environmental consequences. A better understanding of WAS composition is thus very critical for sustainable sludge management. In this work, the occurrence and distribution of several fundamental sludge constituents were explored in WAS samples from nine full-scale wastewater treatment plants (WWTPs) of Beijing, China. Among all the components investigated, active heterotrophic biomass was dominant in the samples (up to 9478 mg/L), followed by endogenous residues (6736 mg/L), extracellular polymeric substances (2088 mg/L), and intracellular storage products (464 mg/L) among others. Moreover, significant differences (p < 0.05) were observed in composition profiles of sludge samples among the studied WWTPs. To identify the potential parameters affecting the variable fractions of sludge components, wastewater source as well as design and operational parameters of WWTPs were studied using statistical methods. The findings indicated that the component fraction of sewage sludge depends more on wastewater treatment alternatives than on wastewater characteristics among other parameters. A principal component analysis was conducted, which further indicated that there was a greater proportion of residual inert biomass in the sludge produced by the combined system of the conventional anaerobic/anoxic/oxic process and a membrane bioreactor. Additionally, a much longer solids retention time was also found to influence the sludge composition and induce an increase in both endogenous inert residues and extracellular polymeric substances in the sludge.     

Rapid detection of multiple class pharmaceuticals in both municipal wastewater and sludge with ultra high performance liquid chromatography tandem mass spectrometry

This work described the development, optimization and validation of an analytical method for rapid detection of multiple-class pharmaceuticals in both municipal wastewater and sludge samples based on ultrasonic solvent extraction, solid-phase extraction, and ultra high performance liquid chromatography-tandem mass spectrometry quantification. The results indicated that the developed method could effectively extract all the target pharmaceuticals （25） in a single process and analyze them within 24 min. The recoveries of the target pharmaceuticals were in the range of 69%-131% for wastewater and 54%-130% for sludge at different spiked concentration levels. The method quantification limits in wastewater and sludge ranged from 0.02 to 0.73 ng/L and from 0.02 to 1.00μg/kg, respectively. Subsequently, this method was validated and applied for residual pharma- ceutical analysis in a wastewater treatment plant located in Beijing, China. All the target pharmaceuticals were detected in the influent samples with concentrations varying from 0.09 ng/L （tiamulin） to 15.24 μg/L （caffeine）; meanwhile, up to 23 pharmaceuticals were detected in sludge samples with concentrations varying from 60 ng/kg （sulfamethizole） to 8.55 mg/kg （ofloxacin）. The developed method demonstrated its selectivity, sensitivity, and reliability for detecting multiple-class pharmaceuticals in complex matrices such as municipal wastewater and sludge.     

城市污水处理厂污泥重金属污染状况及特征

研究了我国16家城市污水处理厂污泥中重金属(Cu,Cr,Pb,As和Cd)污染状况及特征,并探讨了可行的污泥处置方法. 结果显示:w(Cu),w(Cr),w(Pb),w(As)和w(Cd)(干基)分别为14.48～239.93,7.86～200.00,6.10～121.00,3.15～11.70和0.31～6.16 mg/kg;不同种类的重金属在污泥中的质量分数也不同,w(Cu)和w(Cr)高于w(Pb),w(As)和w(Cd);污泥中重金属质量分数还随污水处理厂的不同而变化,这与污水来源和污水处理工艺有关. 分析表明,除7号污水处理厂污泥中w(Cd)超出我国农用泥质(CJ/T309—2009)A级污泥、园林绿化用泥质(GB/T23486—2009)和土地改良用泥质(CJ/T291—2008)中酸性土壤(pH<6.5)施用标准外,其他污水处理厂的污泥重金属质量分数均低于我国农用泥质(CJ/T309—2009)A级污泥标准以及美国、德国和欧盟农用污泥标准的重金属控制限值. 达标的污泥可将混合填埋、农用、园林绿化、土地改良、制砖和水泥熟料生产作为污泥处置备选方案.      

Characterization, treatment and releases of PBDEs and PAHs in a typical municipal sewage treatment plant situated beside an urban river, East China

Characterization, treatment and releases of eight polybrominated diphenyl ethers (PBDEs) congeners and sixteen polycyclic aromatic hydrocarbons (PAHs) in wastewater were evaluated along the treatment processes of a typical secondary treatment municipal sewage treatment plant (STP) (in Hefei City) situated the beside Nanfei River, East China. The findings showed that the average concentrations of the total PBDEs in raw wastewater and treated effluent were 188.578 and 36.884 ng/L respectively. Brominated diphenyl ether (BDE) 209 congener, the predominant PBDE in the STP and Nanfei River, could be related to the discharge of car-industry-derived wastes. For PAHs, the average concentrations in raw wastewater and treated effluent were 5758.8 and 2240.4 ng/L respectively, with naphthalene, benzo[a]pyrene and indeno[1,2,3-c,d]pyrene being detected at the highest concentrations. PAHs mainly originate from the combustion of biomass/coal and petroleum. The STP reduced about 80% of the PBDEs and 61% of the PAHs, which were eliminated mainly by sedimentation processes. The removal rates of PBDEs/PAHs increased with the increase of their solid-water partitioning coefficients. Accordingly, the STP's effluent, containing some PBDE congeners (e.g., BDE 47, 99 and 209, etc.) and low-molecular-weight PAHs, could be an important contributor of these contaminants' input to Nanfei River. It resulted in a significant increase of PBDE/PAH concentrations and PAH toxicological risk in the river water downstream. About 4.040 kg/yr of PBDEs and 245.324 kg/yr of PAHs could be released into the Nanfei River. The current conventional wastewater treatment processes should be improved to remove the relatively low-molecular-weight PBDEs/PAHs more effectively.     

活性污泥二次污染问题的探讨

讨论了城市污水经过A／O工艺处理时活性污泥的二次污染问题。所采用的方法是将原水、处理后的出水及活性污泥用乙酸丁酯萃取、萃取相经过真空浓缩后，采用GC／MS测定了样品中的有机化合物。结果表明，在A／O工艺处理城市污水过程中，活性污泥的吸附作用是主要的，降解作用是次要的：A／O工艺所排放的活性污泥仍然是一种危险的污染物。     

典型医药活性物质在污水处理厂中的归趋及其风险评估

采用固相萃取、高效液相色谱/串联质谱法 (污泥样品先采用超声波萃取预处理方法提取) 检测分析了包括磺胺类、喹诺酮类、大环类酯类抗生素、心血管类、止痛剂类等8类医药活性物质在重庆某污水厂中的含量水平及其行为归趋.采用 EC/PNEC 综合评价体系评估环境中目标医药活性物质的生态风险,利用质量平衡分析的方法分析了其在水相及污泥相中的分布.结果表明,目标物质在水相中均可检出,其检出浓度在ng/L~μg/L,在污泥样品中可检测出18种目标物质,其浓度在ng/g (干重,下同).仅仅1.1%的目标物质被污泥吸附去除.污水处理厂初级处理及氯化消毒阶段对目标物质无明显去除效果,目标物质的去除主要发生在生物处理阶段,生物的降解或转化作用是目标物质的主要去除机制.EC/PNEC分析表明,磺胺嘧啶、磺胺甲恶唑、氧氟沙星与脱水红霉素在污水处理厂出水及其污泥中综合评价因子均大于1,它们的存在可能对环境产生不同程度的危害.本研究结果表明,污水处理厂并不能完全去除水相中微量的医药物质,为防止排放导致的潜在生态风险,出水及污泥中活性医药物质需采取措施进行进一步的处理.     

Quantification of hookworm ova from wastewater matrices using quantitative PCR

A quantitative PCR(q PCR) assay was used to quantify Ancylostoma caninum ova in wastewater and sludge samples.We estimated the average gene copy numbers for a single ovum using a mixed population of ova.The average gene copy numbers derived from the mixed population were used to estimate numbers of hookworm ova in A.caninum seeded and unseeded wastewater and sludge samples.The newly developed qP CR assay estimated an average of3.7 × 10~3 gene copies per ovum,which was then validated by seeding known numbers of hookworm ova into treated wastewater.The qP CR estimated an average of(1.1 ± 0.1),(8.6 ± 2.9)and(67.3 ± 10.4) ova for treated wastewater that was seeded with(1 ± 0),(10 ± 2) and(100 ± 21)ova,respectively.The further application of the q PCR assay for the quantification of A.caninum ova was determined by seeding a known numbers of ova into the wastewater matrices.The qP CR results indicated that 50%,90% and 67% of treated wastewater(1 L),raw wastewater(1 L)and sludge(~4 g) samples had variable numbers of A.caninum gene copies.After conversion of the q PCR estimated gene copy numbers to ova for treated wastewater,raw wastewater,and sludge samples,had an average of 0.02,1.24 and 67 ova,respectively.The result of this study indicated that qP CR can be used for the quantification of hookworm ova from wastewater and sludge samples;however,caution is advised in interpreting qP CR generated data for health risk assessment.