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%.     

典型污染区农业土壤中PAHs的分布、来源及生态风险

采用同位素稀释气相色谱-质谱（GC/MS）分析了路桥农业表层土壤中16种优控PAHs的含量,并对其分布、来源及生态风险进行了分析.结果表明,土壤中16种PAHs的检出率达到100%,其总含量范围为52.3~991 μg·kg-1,与土壤有机碳显著相关（p < 0.01）.PAHs组成特征表明,路桥土壤中以高环PAHs为主.PAHs（除Nap、Acy和Fl）间呈显著相关（r > 0.7,p < 0.01）,表明采样区PAHs污染来源具有一定的相似性.同分异构体比值和因子分析表明,路桥农业土壤中PAHs主要来源于煤和生物质的燃烧.土样中16 PAHs的毒性当量浓度（TEQBaP）介于4.61~164 μg·kg-1之间,7种致癌性PAHs对总TEQBaP的贡献达99%.在35%的土样中,10种PAHs的总TEQBaP超过荷兰土壤目标参考值,表明路桥部分农业土壤存在潜在的生态风险.     

滇池流域宝象河水库沉积物中多环芳烃的垂直分布特征及来源解析

采用GC-MS检测了滇池宝象河水库沉积物中16种美国环保署(US EPA)优先控制的多环芳烃(PAHs)的含量,并对其垂直分布特征及来源进行分析,以此了解宝象河水库近年来PAHs的变化.结果表明,水库沉积物中16种PAHs均有检出,其含量范围为162.26~762.24ng·g~(-1),平均值为423.30 ng·g~(-1).自底层50 cm至表层,沉积物中PAHs含量呈上升趋势.从多环芳烃环数来看,沉积物中的PAHs以2~3环为主,其含量为128.34~518.81 ng·g~(-1),平均值为279.88 ng·g~(-1),占PAHs总量的42.2%~84.1%,平均值为67.6%.FLA/(FLA+PYR)、Ba A/(Ba A+CHR)和Icd P/(Icd P+Bghi P)3组比值及PAHs各组分的分析结果表明,燃烧过程是沉积物中PAHs的主要来源,主要为煤炭、生物质的燃烧.PAHs含量与总有机碳(TOC)之间有显著正相关关系,TOC影响宝象河水库沉积物中PAHs的分布.     

华北地区城镇多环芳烃干沉降特征

分别于冬季和夏季采集了北京、天津和秦皇岛3个城市,遵化、沧县、涞源和张北4个县城以及两处人为活动较少的背景地区降尘样品,分析了降尘量及降尘中多环芳烃含量,据此计算了各样点多环芳烃干沉降通量.结果表明,所研究城市夏季和冬季多环芳烃平均沉降通量分别为(6.3±7.4)μg·m-2·d-1和(16.4±14.9)μg·m-2.d-1,县城为(2.2 4±0.9)μg·m-2 d-1和(16.3±3.8)μg·m-2·d-1,对照点明显低于城镇,两季多环芳烃沉降通量分别为(1.0±0.3)μg·m-2 d-1和(1.6 4±0.7)μg·m-2,d-1.两季节获得的所有样点多环芳烃干沉降通量与降尘量显著相关,若分季节统计,相关性更加明显,且冬季降尘中多环芳烃含量显著高于夏季.由此可见,对多数样点而言,导致其多环芳烃干沉降通量差别的首要因素是降尘量,其次为季节差异.仅个别数据(夏季秦皇岛)表现出不同.降尘中多环芳烃成分谱具有明显的季节差异,城市与县城冬季降尘中菲的相对含量显著高于夏季.不同类型样点间差别较小,表现出区域性趋同现象,同种类型样点之间的多环芳烃成分谱则非常一致.     

水稻根系中多环芳烃的动态变化

水稻根系的多环芳烃浓度随着水稻的生长不断变化,呈现出初期逐渐升高,到成熟期趋于稳定的一般趋势.幼穗期、乳熟期、蜡熟期、完熟期和枯熟期水稻根系的多环芳烃总含量(PAH15)平均分别为464、969、592、1075 ng·g-1和1059ng·g-1,并主要由3环化合物组成.根系的脂含量、比表面和生物量等指标对根系多环芳烃的变化起到了一定影响.其中,脂含量和比表面的影响比生物量的影响更为显著.随着水稻的成熟,水稻土多环芳烃含量逐渐降低,而5、6环化合物的比例逐渐增加.水稻根系和水稻土中的多环芳烃含量之间存在明显的负相关关系.     

选择性吸附法处理含表面活性剂和多环芳烃的土壤淋洗液研究

比较研究了H103树脂、活性炭、沸石、硅藻土和膨润土等5种吸附剂对土壤淋洗液中TX-100与PAHs的吸附性能.批实验结果表明,H103树脂、活性炭、沸石、硅藻土和膨润土吸附后,淋洗液中T-PAHs及TX-100浓度分别为0.03和0 mg·L~(-1)、0.16和3623 mg·L~(-1)、15.21和6175 mg·L~(-1)、15.98和6555 mg·L~(-1)、9.49和4332 mg·L~(-1),选择性吸附系数排序依次为活性炭膨润土沸石硅藻土H103树脂.其中,活性炭能够去除淋洗液中99%的PAHs,同时保留51.33%的TX-100回收再利用,选择吸附系数达到109.5.活性炭固定床实验中,由淋洗液溶质的穿透曲线计算出物质的吸附容量.当空隙体积为2.5-7PV时,活性炭能够去除淋洗液中72%的PAHs,同时保留81%的TX-100,平均选择吸附系数为10.08.由此可见,活性炭固定床可有效处理含表面活性剂土壤淋洗液中的多环芳烃,同时实现表面活性剂的回收再利用.     

胶州湾表层沉积物中多环芳烃的分布及来源

利用气相色谱-质谱方法对胶州湾沉积物中23种多环芳烃(PAHs)进行了分析测定。结果表明，PAHs的总含量范围为82～4567ng／g。PAHs总量在表层沉积物中总趋势是东部高于西部，以东岸附近处最大，远离东岸浓度降低，在胶州湾人海口处最低。造成这种格局的原因有：(1)绝大部分污染源集中在胶州湾东岸；(2)胶州湾的环流系统使东部的污染物很难向西部扩散；(3)沉积物粒度及有机质含量对PAHs含量分布有一定的影响。P／A、PL／PY比值、PAHs环数以及烷基化PAHs表明胶州湾表层沉积物中PAHs几乎全部由人类活动产生，来源为煤炭、木材燃烧、石油类高温裂解及油类污染。与国内外同类研究结果相比，判定为中等污染水平。     

珠江三角洲一些菜地土壤中多环芳烃的含量及来源

为了探讨珠江三角洲中心区经济发达地带的多环芳烃污染水平,为有关部门制定相关的环保政策提供依据,分析了55个分别采自广州、东莞以及佛山郊区表层菜地中土壤样品的多环芳烃的含量.16种EPA(美国环保署)规定的优先控制多环芳烃含量为58～3077 μg·kg-1,均值为315 μg·kg-1,相对于土壤标准和世界其它地区的检测结果属于中等程度污染.分析结果表明,土壤中多环芳烃的含量同土壤总有机碳、碳黑存在着显著的线性关系.通过几个常用参数分析得知,广州、东莞及佛山的多环芳烃污染来源于石化污染以及化石燃料、生物质和煤炭的燃烧.据估算,广州、东莞及佛山0～20 cm表层土壤中多环芳烃类的储量为1292t.     

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.     

北京PM2.5中多环芳烃的污染特征及来源研究

采用GC/MS定量分析了2003年9月至2004年7月期间北京市PM2.5中16种优控PAHs的含量.研究表明.PAHs总浓度年均值139.59ng·m-3,变化范围1.02-776.4 ng·m-3.冬季浓度最高271.05 ng·m-3,夏季最低26.10 ng·m-3,反映了主要源排放(燃煤)变化与气象条件的共同影响.全年平均不同环数PAHs所占总浓度的比例由大到小:4环>5环>6环>3环>2环;冬季4环PAHs所占比例最大(48.7%),其次为5环(32.5%)和6环PAHs(14.9%);夏季5环、6环PAHs所占比例最高(36.5%),其次为4环PAHs(24.1%).源排放特征化合物比值法和主成分分析法结果都表明,燃煤、机动车和油类挥发是多环芳烃的3类主要污染源,能够解释主成分分析法总方差的88%.     

南黄海中部表层沉积物中多环芳烃分布特征及来源分析

通过对南黄海中部49个表层沉积物样品进行总有机碳,粒度,多环芳烃和甲基菲等GS-MS定量分析,探讨了研究区沉积物中多环芳烃分布特征,分子组成,评估南黄海中部多环芳烃污染水平并识别其来源.研究表明,南黄海中部14种多环芳烃总量(ΣPAHs)在81.63~6567.31 ng/g之间,其中优控多环芳烃(ΣEPA PAHs)11种,含量为29.2~1029.1 ng/g,平均含量255.1 ng/g,与国内外其他地区相比有机污染水平为中-低;苝为研究区内主要多环芳烃,分布较为广泛,其含量占所有PAHs的6.40%~88.85%,低含量苝与人为活动有关,而高含量苝代表了陆源有机质输入;多环芳烃组成,异构体分析和甲基菲特征表明,研究区优控多环芳烃主要为煤和高等植物燃烧或不完全燃烧产物以气溶胶形式输入,但部分样品表现出明显的石油源特性也证实了石油燃料,原油泄露产生的多环芳烃客观存在.     

煤矸石堆放对土壤环境PAHs污染的影响

为探讨煤矸石堆放对土壤环境的有机污染效应,以典型煤矸石区——平煤十二矿为例,利用GC-MS技术对煤矸石、表层土壤及降尘样品中多环芳烃(PAHs)含量及化学组成特征进行了检测,将PAHs空间分布、环数分布、优势组成与分子标志物参数相结合,定性剖析了煤矸石堆放对表层土壤PAHs污染的贡献.煤矸石、降尘和土壤表层中PAHs综合分析表明,煤矸石堆积区表层土壤US EPA 16种优控PAHs(PHA₁₆)总量为0.94~5.66 μg·g^-1,属严重污染;表层土壤PAH₁₆总量与煤矸石山距离呈负相关关系;煤矸石、降尘及表层土壤中PAHs均为富3环特征,以菲、苯并荧蒽、、荧蒽及芘为优势组成;煤矸石扬尘直降、煤矸石燃烧、原煤煤尘降落和燃烧对土壤环境PAHs均有输入,但近源区煤矸石扬尘直降贡献明显,煤矸石扬尘使煤矿区土壤环境中PAHs污染具有面源贡献的特点,应引起重视.     

Mixed uncertainty analysis of polycyclic aromatic hydrocarbon inhalation and risk assessment in ambient air of Beijing

This article presents the application of an integrated method that estimates the dispersion of polycyclic aromatic hydrocarbons (PAHs) in air, and assesses the human health risk associated with PAHs inhalation. An uncertainty analysis method consisting of three components were applied in this study, where the three components include a bootstrapping method for analyzing the whole process associated uncertainty, an inhalation rate (IR) representation for evaluating the total PAH inhalation risk for human health, and a normally distributed absorption fraction (AF) ranging from 0% to 100% to represent the absorption capability of PAHs in human body. Using this method, an integrated process was employed to assess the health risk of the residents in Beijing, China, from inhaling PAHs in the air. The results indicate that the ambient air PAHs in Beijing is an important contributor to human health impairment, although over 68% of residents seem to be safe from daily PAH carcinogenic inhalation. In general, the accumulated daily inhalation amount is relatively higher for male and children at 10 years old of age than for female and children at 6 years old. In 1997, about 1.73% cancer sufferers in Beijing were more or less related to ambient air PAHs inhalation. At 95% confidence interval, approximately 272–309 individual cancer incidences can be attributed to PAHs pollution in the air. The probability of greater than 500 cancer occurrence is 15.3%. While the inhalation of ambient air PAHs was shown to be an important factor responsible for higher cancer occurrence in Beijing, while the contribution might not be the most significant one.     

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...     

Evidence of temperature-controlled dissolved inorganic nitrogen distribution in a shallow lake

Dissolved inorganic nitrogen (DIN) plays an important role in aquatic ecosystems as an available source of nitrogen (N). Despite recent advances in our understanding of the effects of climate change on DIN in coastal waters, shallow high-latitude lakes exposed to large seasonal temperature differences have received limited research attention. Therefore, in the present study, Baiyangdian Lake (BYDL) was selected as the study area, as a typical high latitude shallow lake in North China. Based on water and sediment samples collected in spring, summer and winter seasons, DIN accumulation in sedimentary pore water and DIN diffusion fluxes at the sediment-water interface were quantified under different temperature conditions. Correlation analysis was used to establish the effects of temperature on DIN concentration and diffusion in different media. Results show that the diffusion of DIN at the lake sediment-water interface exhibited a strongly positive relationship with temperature, suggesting that high temperature conditions lead to greater DIN release from sediments. Cold temperatures cause DIN accumulation in sedimentary pore water, providing sufficient substrate for N-related bacteria in the sediment under cold temperature conditions. Temperature controls the vertical distribution of DIN by affecting its migratory diffusion and transformation at the sediment-water interface. These findings are valuable for understanding the impact of climate change on the distribution of N in inland shallow lakes, especially in high latitude shallow lakes subjected to large seasonal temperature differences throughout the year.     

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.     

西藏色季拉山公路沿线PAHs分布、来源及风险

分别于2017年3月和12月沿色季拉山318国道采集表层土和冷杉（Abies Mill.）样品,测定了多环芳烃（PAHs）的含量.表层土和冷杉叶中∑₁₆PAHs的含量范围分别为30.21~366.94ng/g dw和39.53~236.42ng/g dw,组成以低环（2、3环）为主.通过特征单体比值法和主成分分析法分析表明,色季拉山PAHs主要来源于化石燃料和生物质的燃烧,同时也受到车辆石油泄漏和大气远距离传输的影响;通过反向气团轨迹判断,色季拉山PAHs大气传输污染主要来自于印度次大陆.色季拉山公路沿线土壤中PAHs的终生致癌风险值均低于1×10^-6,说明对当地居民的致癌风险较小.     

滹沱河冲洪积扇深层孔隙水中多环芳烃和酞酸酯的污染水平与饮水健康风险评估

2015年2月采集石家庄地区滹沱河冲洪积扇深层孔隙水地下水水样,采用气相色谱-质谱法测定了US EPA优先控制的多环芳烃（PAHs）和酞酸酯（PAEs）,并对PAEs的饮水健康风险进行了评估.结果显示,7个采样点均检出PAHs和PAEs,∑PAHs范围为34.4~598.5ng/L,且2~3环PAHs的质量分数介于50%~83%;∑PAEs范围为27.6~25236.7ng/L,其中有3个点位∑PAEs达到20μg/L水平,且7个点位均以DBP、DEHP为主.与国内其他研究区相比,本研究区∑PAHs浓度与国内非岩溶地下水的污染水平接近,而∑PAEs浓度较高.饮水健康风险评估结果显示,仅G2点位的PAHs终生致癌风险指数小于US EPA推荐的可接受的水平（10^-6）,其致癌风险可以忽略外,其他点位均具有潜在致癌风险;而对于PAEs饮水终生致癌风险而言,G1、G6、G73个点位的PAEs终生致癌风险也均高于10^-6,因此,研究区深层孔隙水中的PAHs和PAEs污染均应当引起重视.     

煤矿矿区土壤重金属及多环芳烃污染治理修复技术综述

土壤重金属和有机物污染是当前许多煤矿矿区及周边地区面临的严重问题,威胁居民健康,要采取有效措施予以解决。在对煤矿矿区周边土壤重金属和多环芳烃（PAHs）来源及危害分析的基础上,发现重金属元素在自然条件下难以降解,导致其在生物体中累积,并且PAHs具有致癌性、致畸性和诱变性。通过比较物理化学修复、植物修复和生物修复等方法在治理重金属及PAHs污染土壤的优缺点,发现植物修复和生物修复对气候和环境的依赖程度高,物理修复成本和能耗较高,因此提出矿区周边土壤污染的修复技术需要进一步创新,实现多领域、多学科协作发展的观点。通过持续的技术创新和多种修复方法的联合应用,达到有效治理煤矿矿区及周边重金属和PAHs污染的目的,实现土壤的重新利用,进而实现环境保护与经济可持续发展的良性互动。

     

慈溪市农田表层、亚表层土壤中多环芳烃(PAHs)的分布特征

为了解多环芳烃在土壤中的迁移,研究了慈溪市农田表层土壤(耕层)和亚表层(犁底层)土壤中15种PAHs的含量及分布特征.表层土壤中PAHs的总量在70.4～325.1μg·kg-1之间;含量较高的几种化合物为萘(Nap)、菲(Phe)、荧葸(na)、芘(pyr)和苊(her)等,但主要以4环以上芳烃为主;Fla/(Fla Pyr)与IcP/(IeP BgP)比值分析表明,表层土壤中的PAHs主要来源于草、木、煤等的燃烧和汽车尾气排放.亚表层土壤中,PAHs总量为29.5～232.3μg·kg-1,以2环加3环化合物为主,单体PAH含量与表层土壤中含量的比值与其辛醇-水分配系数(10gKow)显著相关(r=0.923,P＜0.0001),说明亚表层土壤中PAH主要来源于表层土壤的淋溶,根据化合物的logKow值可预测其在土壤中的迁移情况.亚表层土壤中PAHs的含量与有机质的含量极显著相关(r=0.945,P＜0.0001),但表层中二者则无显著相关性(p=0.0887),表明耕作措施可能会对PAH在表层土壤中的分布产生影响.