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.     

大辽河水系表层沉积物中石油烃和多环芳烃的分布及来源

对大辽河水系的3条干流浑河、太子河和大辽河表层沉积物中石油烃(PHs)和多环芳烃(PAHs)分析表明,PHs总量分布范围为61.37～229.42 μg·g-1,PAHs总量分布范围为61.9～840.5 ng·g-1.石油烃含量远远高于已报道的世界其它河流和海洋沉积物中的含量,表明大辽河水系沉积物石油烃污染严重;而与世界其它河流和海洋地区相比,多环芳烃污染水平相对偏低.石油烃分布特征为太子河＞浑河＞大辽河;多环芳烃分布特征为大辽河＞太子河＞浑河.烃污染来源诊断表明,石油烃污染以陆源植物和人为污染输入为主,多环芳烃污染以石油燃烧热解为主,工业和生活污水是烃污染的主要来源.     

我国大气背景点颗粒物PAHs分布特征及毒性评估

选择我国自北向南4个国家大气背景监测站(吉林长白山、山西庞泉沟、湖北神农架和广东南岭),于2013年4个季度采集了环境空气PM2.5和PM10样品,采用超声波乙腈萃取-超高压液相色谱分析16种多环芳烃.结果表明,4个大气背景点的PM2.5和PM10中∑PAHs浓度分别为0.09~25.42ng/m3和0.13~30.16ng/m3,与国内外大气背景点基本处于同一浓度水平,空间分布特点为庞泉沟>长白山>神农架>南岭,季节分布特点为庞泉沟和神农架春季、冬季,长白山的春季,以及南岭冬季明显高于所在背景点的其他季节.PM2.5和PM10中BaP和∑PAHs在低浓度范围内均呈现显著的线性相关性.除了长白山冬季和南岭夏季的3环PAHs比例较高外,其余季节的背景点以4环和5环PAHs为主,主要为荧蒽、芘、苯并(a)荧蒽.通过BaP当量进行了致癌性和致突变性评价,结果显示庞泉沟春季和冬季颗粒物的∑BaPTEF和∑BaPMEF相对较高,分别为1.81~2.74ng/m3和2.92~4.36ng/m3, 对所在区域的PAH污染状况需要关注.     

Seasonal variation and sources of atmospheric polycyclic aromatic hydrocarbons in a background site on the Tibetan Plateau

The study of atmospheric polycyclic aromatic hydrocarbons (PAHs) in northeastern Tibetan Plateau with fragile ecological environment and complex atmospheric circulation system is blank. To understand the characteristics and sources of persistent organic pollutants in the atmosphere of the northeastern Tibetan Plateau, we monitored levels in the central Qilian Mountain. From 2016 to 2017, we collected 45-pair (particle + gas) samples using active air samplers to investigate the sources, transport paths, and their influencing factors. Sources of PAHs were analysed with a source diagnostic model, and atmospheric transport paths were calculated. The concentration range for ∑₁₅PAHs was 439–4666 pg/m³, and the average was 2015 pg/m³. The PAHs in central Qilian Mountain are mainly low molecular weight (LMW) PAHs. Winter concentrations of PAHs were higher than those in summer. The transport of PAHs is mainly affected by westerlies, and there are seasonal differences. Source analysis showed that PAHs mainly came from coal and biomass combustion and vehicle emissions, with seasonal differences. This study clarifies the concentration and seasonal variation of PAHs in the northern Tibetan Plateau, which is conducive to understanding the atmospheric transport process and fate of pollutants. The background site of Qilian Mountains located in the Silk Road economic belt has the value and significance of long-term observation of pollutants.     

成都市PM10中多环芳烃来源识别及毒性评估

对成都市2009年冬夏两季可吸入颗粒物(PM10)中16种多环芳烃(PAHs)含量进行了研究,并进一步分析其空间分布、组成特征及来源.结果表明,16种PAHs中15种被普遍检出(Nap未检出),冬季和夏季的ΣPAHs浓度范围分别为40.25~150.68ng/m3和44.51~71.16ng/m3,平均浓度分别为88.36ng/m3和64.21ng/m3.空间分析表明,PAHs浓度在工业区较高,背景点较低.从PAHs组分分析结果显示,低环含量较低,4~6环所占比例较大,其比例范围为86.7%~96.1%.各组分含量季节差异不明显.利用特征化合物比值法、等级聚类法、PCA解析法分析了污染源类型,结果表明成都市PM10中PAHs的主要来源是机动车尾气排放源,以及煤与木材燃烧源.通过BaP当量(BaPE)进行了毒性评估,结果显示成都市冬夏两季的BaPE均值分别为13.41ng/m3和9.54ng/m3.     

象山港海水和沉积物中多环芳烃分布特征和来源研究

本文研究了象山港多环芳烃（PAHs）在沉积物-海水中的分布特征,于2017年1月对港口9个采样点的沉积物和海水中16种优先控制PAHs进行分析,采用同分异构比值法和逸度方法进行来源分析和扩散行为研究。沉积物中PAHs范围为17.51×10–9～84.41×10–9,主要为高环PAHs,处于轻度污染等级。沉积物中多环芳烃主要来自高温燃烧源。表层水体、中层水体和底层水体中PAHs范围分别为41.78～105.72 ng/L、41.51～106.34 ng/L和9.18～145.17 ng/L,主要由低环PAHs组成。表层水体中PAHs主要来源于石油泄漏和石油燃烧。利用逸度系数判断PAHs扩散行为,萘（Nap）、苊（Ace）和芴（Flo）由沉积物向海水释放;苊烯（Acy）、菲（Phe）、蒽（Ant）和芘（Pyr）在沉积物和海水中处于动态平衡;荧蒽（Flu）、苯并[a]蒽（BaA）、?（Chr）和苯并[b]荧蒽（BbF）主要从海水向沉积物扩散并富集。     

Pollution characteristics, sources and lung cancer risk of atmospheric polycyclic aromatic hydrocarbons in a new urban district of Nanjing, China

This paper focused on the pollution characteristics,sources and lung cancer risk of atmospheric polycyclic aromatic hydrocarbons(PAHs) in a new urban district of Nanjing,China.Gaseous and aerosol PM_(2.5)(particulate matter with aerodynamic diameter smaller than2.5 urn) samples were collected in spring of 2015.Sixteen PAHs were extracted and analyzed after sampling.Firstly,arithmetic mean concentrations of PAHs and BaP_(eq)(benzo[a]pyrene equivalent) were calculated.The mean concentrations of PAHs were 29.26±14.13,18.14±5.37 and 48.47±16.03 ng/m~3 in gas phase,particle phase and both phases,respectively.The mean concentrations of BaP_(eq) were 0.87±0.51,2.71±2.17 and 4.06±2.31 ng/m~3 in gas phase,particle phase and both phases,respectively.Secondly,diagnostic ratios and principal component analysis were adopted to identify the sources of PAHs and the outcomes were the same:traffic exhaust was the predominant source followed by fuel combustion and industrial process.Finally,incremental lung cancer risk(ILCR) induced by whole year inhalation exposure to PAHs for population groups of different age and gender were estimated based on a Monte Carlo simulation.ILCR values caused by particle phase PAHs were greater than those caused by gas phase PAHs.ILCR values for adults were greater than those for other age groups.ILCR values caused by total(gas + particle) PAHs for diverse groups were all greater than the significant level(10~6),indicating high potential lung cancer risk.Sensitivity analysis results showed that cancer slope factor for BaP inhalation exposure and BaP_(eq) concentration had greater impact than body weight and inhalation rate on the ILCR.     

城市大气中多环芳烃的降雨冲刷

2009年7~8月采集了10场降雨的雨水及对应降雨前后的大气样品,研究降雨对大气中多环芳烃的冲刷和净化作用.雨水中多环芳烃以颗粒态为主,4环组分浓度最高.气态、颗粒态和总的多环芳烃的净化率分别为3.9×102、3.7×104和5.9×103.降雨对大气的冲刷以颗粒物为主,气态多环芳烃的净化主要体现为低环组分(2~3环),高环(4~6环)组分主要以颗粒态的形式进行冲刷和净化,总净化率4~6环组分PAHs高于2~3环组分.大气颗粒态PAHs和气态PAHs的降雨沉降效率与包括降雨时间等在内的降雨综合特征有显著相关关系.     

泛杭州湾海域沉积物中多环芳烃分布及源解析

2011~2014年每年对泛杭州湾海域36个站位采集表层沉积物样品,对沉积物样品中16种多环芳烃（PAHs）的含量进行检测,了解其浓度水平、空间分布特征以及组成结构,并通过结构组成进行来源解析。结果表明,2011~2014年该海域沉积物中PAHs处于中度污染水平,平均含量及其标准偏差分别为（116.03±15.26）×10-9、（106.59±13.90）×10-9、（129.05±14.37）×10-9、（106.10±10.43）×10-9。空间分布上,PAHs高值区主要集中于长江口以及舟山海域附近,近岸区域高于远岸区域,远岸区有个别相对高值区。单体PAH中,菲的含量最高,环数主要分布在3~5环,以高分子量为主;来源解析结果表明污染源主要是煤、木柴和生物质的燃烧,部分站位同时受到石油源影响。     

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.     

上海市大气沉降物中多环芳烃赋存特征及其来源

以上海市大气沉降为研究对象,采集了上海市8月、9月、10月3个月的大气沉降物,分析了上海市大气沉降物中16种PAHs的质量浓度、空间分布特征和组成结构,计算了上海市8个采样点∑15PAHs大气沉降物通量.同时,采用正定矩阵因子分解(PMF)模型对大气沉降中的PAHs进行源解析,模型对PAHs的来源有较为细致的判读,结果表明:大气沉降物中∑16PAHs的浓度范围0.458~21.013μg/L,其中,溶解相中∑16PAHs的浓度范围为0.174~0.625μg/L,颗粒相中∑16PAHs的浓度范围为0.275 20.455μg/L.上海市∑15PAHs大气沉降通量在0.24~14.74μg/(m2×d)之间,沉降通量均值为2.77μg/(m2×d).根据PMF模型解析,机动车尾气排放为大气沉降物中PAHs的主要污染物,源贡献率为40.23%,其次,居民烹调、煤炭燃烧、石油挥发泄露和炼焦排放依次占23.73%、14.75%、14.35%和6.92%.     

Diurnal variation of nitrated polycyclic aromatic hydrocarbons in PM10 at a roadside site in Xiamen, China

Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons (NPAHs) in PM₁₀ at a roadside site in Xiamen, China. At the same time, six PM₁₀ samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2-and 3-nitrofluoranthene, 1-nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs (∑NPAHs) in the cold season (26 Nov-31 Dec) was 2.3 (daytime) and 9.9 (nighttime) times higher than those in the warm season. Significant statistical difference (p < 0.01, 2-tailed) of ∑NPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 + 3-nitrofluoranthene to 1-nitropyrene exhibited a similar diurnal pattern as ∑NPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.     

Distribution and sources of polycyclic aromatic hydrocarbons in the water column of Kongsfjorden, Arctic

Kongsfjorden is known for its characteristic multi-layer water mass formed by the convergence of freshwaters from nearby glaciers and rivers and saline water from the Atlantic and Arctic. The distribution of polycyclic aromatic hydrocarbons(PAHs) in the water column of Kongsfjorden was investigated and their potential sources were analyzed. The total concentrations of 16 PAHs in the surface seawater and river water were in the range of 33.4-79.8 ng/L(mean 48.5 ng/L) and 2.3-201.4 ng/L(mean 126.1...     

长江武汉段水体中多环芳烃的分布及来源分析

对长江武汉段干流7个站点、支流和湖泊23个站点的水相、悬浮颗粒相和沉积相样品中的多环芳烃进行了分析测定.结果表明,水相中多环芳烃总量的变化范围为0.242～6.235μg·L-1沉积相中的变化范围为31-4812μg·L-1悬浮颗粒相中多环芳烃含量的平均值为4677μg·L-1,含量高于沉积物.长江武汉段与国内其它河流多环芳烃污染水平相当,比国外一些河流多环芳烃的污染水平要高.沉积相中多环芳烃的含量与颗粒物中总有机碳(TOC)含量呈显著正相关.污染来源分析表明,多环芳烃主要由化石燃料、木材等的燃烧所引起,污染来源为燃烧源.在干流白沙洲和支流墨水湖的水相中检出了苯并(a)芘,且含量超出了国家饮用水标准.沉积物中PAHs对周围生物存在潜在的毒性效应,但不会引起急性毒性效应.     

Source and deposition of polycyclic aromatic hydrocarbons to Shanghai, China

Despite recent efforts to investigate the distribution and fate of polycyclic aromatic hydrocarbons (PAHs) in air, water, and soil, very little is known about their temporal change in wet deposition. As a result of increased attention to public health, a large-scale survey on the deposition flux and distribution of PAH contamination in rainwater was urgently conducted in Shanghai, China. In this study, 163 rainwater samples were collected from six sites, and 15 PAH compounds were detected by the use of a simple solid phase microextraction (SPME) technique coupled with gas chromatography-mass spectrometry. The dominant PAH species monitored were naphthalene, phenanthrene, anthracene, and fluoranthene. The concentration of total PAHs per event was between 74 and 980 ng/L, with an average value of 481 ng/L, which is at the high end of worldwide figures. The annual deposition flux of PAHs in rainwater was estimated to be 4148 kg/yr in the Shanghai area, suggesting rainfall as a major possible pathway for removing PAHs from the atmosphere. Diagnostic analysis by the ratios of An/178 and Fl/Fl+Py suggested that combustion of grass, wood, and coal was the major contributor to PAHs in the Shanghai region. Back trajectory analysis also indicated that the pollutant sources could be from the southern part of China.     

生物源表面活性剂对焦化土壤中多环芳烃增溶效能研究

考察了单一生物源表面活性剂鼠李糖脂、黄腐酸、槐糖脂、烷基糖苷、无患子皂苷及鼠李糖脂与各非离子生物源表面活性剂复配体系对萘和菲的增溶效能,并将优选的淋洗剂体系应用于焦化场地土壤多环芳烃（PAHs）的去除.结果表明：相较其他生物源表面活性剂,鼠李糖脂和黄腐酸对萘的增溶效果更好;对于菲的增溶,槐糖脂的增溶效果更好,这与其较低的临界胶束浓度和多环芳烃的性质有关.生物源表面活性剂复配体系的增溶能力较单一表面活性剂明显增强,以3∶1复配时增溶效果最佳.60 mmol·L^-1的鼠李糖脂-黄腐酸复配体系（3∶1）对土壤中萘的去除率可达96.64%,分别是单一鼠李糖脂和黄腐酸的1.09倍和2.21倍;而对土壤中蒽、苯并（a）蒽和苯并（k）荧蒽的去除率远低于萘,分别为63.31%、42.51%和39.10%,这是由于PAHs与鼠李糖脂-黄腐酸复配体系的相互作用随苯环数的增加而减弱.本研究可为生物源表面活性剂及其复配体系高效修复PAHs污染土壤提供科学依据.     

广州市大气中颗粒态多环芳烃(PAHs)的主要污染源

采用特征化合物与因子分析对广州市大气中颗粒态PAHs的来源及其贡献率进行研究.结果表明,广州大气中颗粒态多环芳烃主要来源是机动车尾气排放和燃煤,其中机动车为主要污染源,占了69%,其次为燃煤,占了31%.冬季大气中颗粒态多环芳烃污染加重的主要原因为低温、无风的气象条件下形成的逆温效应,主要污染源为机动车的尾气排放;夏季颗粒态多环芳烃污染的增大同样是无风时不利于污染物扩散的结果,但此时燃煤对大气中颗粒态多环芳烃污染的贡献要略大于机动车尾气排放.     

兰州市大气颗粒物多环芳烃的恒能量同步荧光光谱特征研究

通过传统单波长激发/发射荧光光谱法与恒能量同步荧光光谱法进行对比,对大气颗粒物中多环芳烃(PAHs)进行了定性定量分析,采用恒能量同步荧光光谱法在不同能量差下建立了15种典型PAHs成分的恒能量同步荧光法的标准谱库.在各PAHs在最佳能量差下进行定量分析,结果表明,除苊荧光信号响应较差外,其余PAHs的LOD和LOQ分别为0.0580～3.18、0.232～12.7 ng·mL~(-1).15种PAHs的空白和一定浓度下的加标回收率范围在82.8%～120.0%,相对标准偏差范围在0.51%～5.87%之间,以恒能量同步荧光光谱进行了兰州地区大气颗粒物中15种PAHs分布特征分析.     

多环芳烃的微生物降解与生物修复

生物修复在治理多环芳烃污染环境中的作用日益突出，其应用越来越受到重视。文中概述了生物修复技术发展的基础－多环芳烃微生物降解，论述了降解微生物分离、驯化、咱类、降解机制等，探讨了提高多环芳烃降解速率的途径及其存在的一些问题，并对今后的发展进行了展望。     

Distribution and origin of polycyclic aromatic hydrocarbons in surface sediments from an urban river basin at the Metropolitan Region of Curitiba, Brazil

The concentrations of 16 polycyclic aromatic hydrocarbons (PAHs) were determined in surface sediment samples from nine sites located at the Iguac?u River Basin in the Metropolitan Region of Curitiba, Brazil to evaluate their distribution and sources. The total concentration of the PAHs was greater for sediments from highly urbanized areas, while the sediments from the Ira′? Environmental Protection Area (Ira′? EPA) showed significantly low concentrations. The sediments from the Iguac?u and Barigui rivers were classified as highly contaminated, while those from the Cercado and Curralinho rivers were classified as moderately contaminated. The predominance of PAHs containing two to four aromatic rings in most of the samples suggested the direct input of raw sewage into the water resources evaluated. Benzo[g,h,i]perylene, dibenzo[a,h]anthracene and indeno[1,2,3-cd]pyrene were predominant in sediments from the areas under the greatest urban and industrial development. The correlation between thermodynamic stability and the kinetics of evolution presented by the isomeric pairs indicated that combustion is the predominant source of PAHs in the sediments because the combustion of fossil fuels affected most of the points evaluated, followed by combustion of biomass and eventually combustion of oil product inputs. In general, the results showed that areas under strong urban influence, as well as the Ira′? EPA, receive contributions of PAHs from similar sources.