钢铁厂及其周围环境中二噁(口英)和多氯联苯土-气交换研究

利用逸度模型及其相关算法,研究了东北某钢铁厂及其周围居住区、背景对照区二噁(口英)和多氯联苯污染物土-气迁移方向和交换通量。结果表明,二噁(口英)主要由大气向土壤迁移,其土-气交换通量为每月618～5373mg/km2,多氯联苯污染物主要由土壤向大气迁移,交换通量为每月47～230mg/km2。基于实测污染物的浓度和逸度模型能较好地估算该地区二噁(口英)、多氯联苯等持久性有机污染物的土-气界面迁移规律。     

2003—2018年全国酸雨状况变化趋势研究

基于2003—2018年全国291个城市降水监测结果的分析表明:全国降水酸度明显降低,其中,2003—2006年有所升高,2006年之后呈降低趋势；酸雨区面积呈减小趋势,共减少约97万km²,酸雨发生频率超过5%的面积减少了20.9个百分点；全国酸雨城市比例为21.3%～40.9%,2009年开始总体呈下降趋势,2018年降为21.6%,重酸雨城市比例在2005年之后总体呈下降趋势；全国平均酸雨频率为11.7%～25.6%,2006年之后总体呈下降趋势,2018年酸雨频率在50%以上的城市比例较2006年下降了13.9个百分点。基于174个城市的降水离子组分分析结果显示:我国降水中的主要阴离子为硫酸根,其离子当量浓度占比为19.4%～32.9%,2003年以来年平均降低0.6个百分点；降水中的主要阳离子为钙离子和铵离子；硫酸根沉降通量年平均下降0.68 t/km²,硝酸根沉降通量年平均降低0.05 t/km²,全国SO₂浓度变化趋势与硫酸根沉降通量变化趋势基本一致；我国降水中的硝酸根与硫酸根离子当量浓度比值总体呈升高趋势,表明硝酸根离子对降水酸度的影响逐渐增加,酸雨类型正由硫酸型向硫酸-硝酸混合型转变。     

干旱区中小城市降雪中金属元素沉降通量研究

文章以干旱区中小城市昌吉市为研究区，选择2011年12月至2012年2月期间较为典型的6场次降雪进行采样，利用ICP-MS测定降雪中20种金属元素，并探讨金属元素的沉降通量、富集特征及其来源。研究表明，降雪中Al的年沉降通量最大，为10.32 mg/m²；Fe、Ba、Zn、V、Cu的年沉降通量次之，集中在1.40~6.11 mg/m²；As、Ni、Mn、Cr、Mo、Sb年沉降通量较小，集中在0.08~0.39 mg/m²；Be、Co、Cd、Pb、Hg、Tl、Th、U的年沉降通量最小，集中在0.001~0.053 mg/m²。Al、Fe、Mn、Be、Th富集系数在0.32~3.05之间，这些金属元素主要来自自然来源；Cd与Hg富集系数分别为923.23、2511.47，达到严重富集的程度；其余金属元素富集系数在10~500之间，属中度富集。昌吉州境内煤炭资源丰富，近年煤炭开采量较大，城区供暖面积不断加大，供暖不断加强；市区车流量急剧增加，运输排放加剧；近郊及周边地区各类工业的分布等是各类金属元素在雪中富集的主要原因。冰雪节后冰灯拆除，降雪可有效捕集大气中的汞，冬季气温不利于Hg挥发等对Hg的严重富集也有重要影响。     

济南市大气细颗粒物中二(口恶)英污染水平及季节变化

2021年对济南市大气PM_2.5中17种2,3,7,8氯取代二(口恶)英(PCDD/Fs)污染现状进行监测。对其异构体分布、指示性单体、季节变化规律等特征及其与常规污染物相关性进行了分析。结果表明:大气PM_2.5中PCDD/Fs浓度范围和年平均值分别为0.157~1.595 pg/m³和0.785 pg/m³,而毒性当量(以I-TEQ计)范围和年平均值分别为0.009~0.116 pg TEQ/m³和0.052 pg TEQ/m³。PCDD/Fs浓度与毒性当量季节变化特征显著,均呈现出冬季>春季>秋季>夏季的情况,可能由季节性排放源和气象条件不同导致。不同季节PCDD/Fs异构体分布模式一致,主要由高氯代(1,2,3,4,6,7,8-HpCDF、OCDD、OCDF和1,2,3,4,6,7,8-HpCDD)单体组成;而对毒性当量贡献最大的单体是2,3,4,7,8-PeCDF,其与总毒性当量具有较好的相关性。同时,PCDD/Fs浓度与SO₂、NO₂、PM_2.5等大气常规污染物呈显著正相关。这表明,大气PM_2.5中PCDD/Fs与常规污染物的生成和排放密切相关。     

污染天气条件下人工降雨对成渝西南区域环境空气质量的影响评估

基于成渝地区大气污染防控形势的严峻性,选取该区域西南部的乐山市作为研究对象,对2016—2020年人工降雨对该城市环境空气质量的影响进行研究。评估发现:冬季改善效果最好,平均每毫米降雨量可降低环境空气质量指数(AQI)约10,对应的SO₂、NO₂、CO、O₃、PM₁₀、PM_2.5浓度分别降低1.8 μg/m³、3.8 μg/m³、0.1 mg/m³、8.1 μg/m³、6.9 μg/m³、8.9 μg/m³;其次是春季,每毫米降雨量可降低AQI约8,对应的6项污染物浓度分别降低1.0 μg/m³、3.3 μg/m³、0.1 mg/m³、8.1 μg/m³、6.1 μg/m³、8.4 μg/m³;再次是夏季,每毫米降雨量可降低AQI约3,对应的6项污染物浓度分别降低0.6 μg/m³、1.6 μg/m³、0.03 mg/m³、6.9 μg/m³、1.2 μg/m³、2.0 μg/m³;秋季每毫米降雨量可降低AQI约1,对应的6项污染物浓度分别降低0.4 μg/m³、0.6 μg/m³、0.01 mg/m³、3.5 μg/m³、0.1 μg/m³、0.1 μg/m³。计算不同季节降雨总量与污染物削减量之间的Pearson相关系数,结果表明,春季人工降雨总量与O₃浓度削减总量呈显著正相关,夏、秋两季人工降雨总量与PM_2.5浓度削减总量呈显著正相关。     

湿法脱硫烟气中多形态颗粒物的测量方法及组分特征

为全面测量固定源湿法脱硫烟气中多形态颗粒物的排放浓度及其离子组成特征，提出了一种基于一级冷凝、二级过滤和一级冲击吸收的多形态烟气颗粒物的同步测量方法，外场实测了3种湿法脱硫和除尘工艺的排放水平。现场测试表明：简易湿法除尘脱硫（NaOH法）一体化装置烟气中可过滤颗粒物（FPM）浓度为（36±11）mg/m³，可逃逸颗粒物（EPM）浓度为（33±7）mg/m³；氧化镁法+布袋除尘工艺烟气中FPM浓度为（14±5）mg/m³，EPM浓度为（13±6）mg/m³；石灰石-石膏脱硫+电袋除尘工艺烟气中FPM浓度低，小于3 mg/m³，EPM浓度为（6±1）mg/m³；烟气中EPM是传统滤膜法检测FPM浓度的0.7~5.7倍，EPM的主要存在形态为冷凝液中的可溶解颗粒物（DPM），颗粒物的组分与脱硫方法密切相关，各形态颗粒物的主要组分是SO₄^2-、SO₃^2-、NO₃^-、NO₂^-、NH₄⁺、Cl^-、Na⁺、Mg²⁺和Ca²⁺等离子。     

莱州湾表层沉积物中多氯联苯的测定方法及分布特征探究

以加速溶剂萃取法 (ASE)、索氏提取法/气相色谱法测定了莱州湾表层沉积物中的12种PCBs的浓度水平,探讨了它的分布特征并将两种方法进行了对比;同时测定了渤海湾北部海域表层沉积物中PCBs的含量,与莱州湾进行了比较。结果表明,莱州湾海域表层沉积物检测出8种多氯联苯(PCBs),浓度范围是N.D.~48.40 ng ·g ^-1dw。该海域多氯联苯的分布特征是近岸高,离岸低,由近岸向湾外延伸方向依次递减;渤海湾PCBs的浓度范围是0.15~68.30 ng ·g ^-1dw,和莱州湾差别不大。索氏提取法测定12种多氯联苯类化合物的基质加标回收率为78.00%~104.85%,相对标准偏差为0.95%~3.64%;加速溶剂萃取法的基质加标回收率为90.00%~102.00%,相对标准偏差为0.65%~2.75%;相对于渤海湾北部海域而言,莱州湾区域只是受到轻度污染,属于低风险生态区,不会对生物产生毒副作用;而前者则处于中度污染水平,可能会对生物产生毒副作用。     

2018年长三角一次持续重污染过程分析

利用常州市6个环境空气质量评价点PM_2.5、PM₁₀、SO₂、NO₂、CO和水溶性离子数据，结合后向轨迹、激光雷达探空资料、气象资料等，分析了2018年1月29日—2月2日长三角区域一次持续重污染过程。结果表明，重度污染时次高达94 h，PM_2.5最高值达235 μg/m³，由外来输送污染物与本地排放的污染物叠加而成，在不利气象条件影响下，污染物在长三角区域长时间滞留；重污染期间，污染物日变化规律显示，PM_2.5受外来源影响更显著，而SO₂、NO₂受本地污染源影响更显著，水溶性粒子组分与常州市本地源存在较大差异，其中NO₃^-、NH₄⁺、K⁺、Mg²⁺和SO₄^2-值增加最为明显，较污染前分别增加了9.1，5.9，4.3，4.2和4.1倍；K⁺值升高较快，说明污染期间也受到了生物质燃烧的影响。此外，NO₃^-和SO₄^2-在空气质量较好时，在水溶性离子中的占比日变化幅度较大，而在重污染期间，NO₃^-和SO₄^2-日变化幅度明显减小。     

云南省臭氧污染特征及气象影响分析

为研究云南省臭氧(O₃)污染特征及其与气象因子的关系,基于统计学方法及ArcGIS空间差异分析、线性趋势分析、空间离散系数等方法,对全省16个市(州)2015—2017年33个环境监测站点的监测数据进行了研究。结果表明:研究期间,O₃逐渐取代其他大气常规污染物成为首要污染物,其浓度变化范围为19～138 μg/m³。云南省各市(州)O₃浓度年变化呈现周期性,月度峰值集中出现在春季(3—5月)；日变化呈单峰形,峰值集中在14:00—17:00。O₃浓度的空间格局由纵向集聚为主转变为横向集聚为主,各集聚区交错分布,低值区由西北部转移到西南部；O₃浓度增长率为正的区域集中于东北部和中部,面积约为20.81万km²,占全省总面积的54.29%,其余半环状区域增长率为负。迪庆州O₃污染情况与其他市(州)明显不同,且受其他市(州)传输的影响较小。气象因子对O₃浓度的影响随时间和地域条件的变化而变化,对典型市(州)(迪庆州、丽江市、昭通市)O₃浓度影响最大的为偏南风,影响的浓度区间为20～160 μg/m³。     

便携式气相色谱-氢火焰离子化检测器法测定低浓度总烃的氧气干扰特征研究

研究了采用便携式气相色谱-氢火焰离子化检测器法测定气体中的总烃浓度时,氧气浓度对测定结果的影响,并采用多元线性回归模型对总烃的测定结果进行了校准。当总烃的实际浓度不低于9 mg/m³时,氧气的干扰较小(相对标准偏差≤2%)。在试验的所有总烃实际浓度下(1~200 mg/m³),当氧气浓度为1%~7%时,也无需考虑氧气干扰的影响(相对标准偏差≤2%)。当总烃的实际浓度低于9 mg/m³且氧气浓度为9%~21%时,需依据多元线性回归分析原理并采用模型对测得的总烃浓度进行校准。线性回归方程分析结果显示,模型拟合情况良好(R²=0.999),可以用来修正测试结果,从而得到更加准确的总烃实际浓度。     

钢铁厂及其周围土壤中二恶英和多氯联苯污染物的分布规律研究

利用同位素稀释高分辨气相色谱-高分辨质谱(HRGC/HRMS)的分析方法研究了东北某钢铁厂及其周围生活区、背景对照区土壤中二噁和多氯联苯污染物的污染水平和分布规律。结果表明,土壤中二噁的浓度和毒性当量分别为26pg/g(6.02～109pg/g)、0.72pg I-TEQ g-1(0.008～5.43pg I-TEQ g-1)。土壤中多氯联苯的浓度为955pg/g(268～3504pg/g),毒性当量值达0.07pg TEQ g-1(0.006～0.33pg TEQ g-1)。该区域土壤中的二噁和多氯联苯浓度明显低于一般国家居住地的土壤控制标准,处于较低的污染水平。     

Contributions of dry and wet depositions of polychlorinated dibenzo-p-dioxins and dibenzofurans to a contaminated site resulting from a penetachlorophenol manufacturing process

The soils at a factory for manufacturing pentachlorophenol were heavily contaminated by polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs). In order to verify the contributions of dry and wet deposition of PCDD/Fs from the ambient air, the concentration of PCDD/Fs in ambient air and soil were measured, the partition of particle- and gas-phases of atmospheric PCDD/Fs was calculated, and the annual fluxes of total dry and wet PCDD/F depositions were modeled. Average atmospheric PCDD/F concentration was 1.24 ng Nm^???3 (or 0.0397 ng I-TEQ Nm^???3). Moreover, over 92.8% of total PCDD/Fs were in the particle phase, and the dominant species were high chlorinated congeners. The total PCDD/F fluxes of dry and wet deposition were 119.5 ng m^???2 year^???1 (1.34 ng I-TEQ m^???2 year^???1) and 82.0 ng m^???2 year^???1 (1.07 ng I-TEQ m^???2 year^???1), respectively. By scenario simulation, the total fluxes of dry and wet PCDD/F depositions were 87.1 and 68.6 ng I-TEQ, respectively. However, the estimated PCDD/F contents in the contaminated soil were 839.9 ?? g I-TEQ. Hence, the contributions of total depositions of atmospheric PCDD/F were only 0.02%. The results indicated that the major sources of PCDD/F for the contaminated soil could be attributed to the pentachlorophenol manufacturing process.     

深圳市大气中PCDD/Fs污染水平初步研究

目的:了解深圳市大气中二噁(PCDD/Fs)的污染水平和分布特征。方法:利用大流量空气采样器分别采集6个采样点的空气样品,每个采样点采集两个平行样品。参照美国环保总局(US EPA Method TO-9A)二噁的检测方法,通过高分辨气相色谱-高分辨双聚焦磁式质谱仪(HRGC/HRMS)对大气样品中17种具有毒性当量因子(TEF)的单体进行了定性和定量分析。结果:∑PCDD/Fs的浓度范围为0.23～11.88pg/m3(平均值为3.84 pg/m3)。毒性当量浓度范围为0.014～0.29 pg I-TEQ/m3(平均值为0.135 pg I-TEQ/m3)。OCDD、HpCDD、HpCDF、OCDF、HxCDF是丰度较大的单体,分别占总浓度的48.21%、15.85%、11.37%、7.40%、6.59%。PCDDs和PCDFs单体浓度(除OCDF之外)均随氯原子取代个数的增加而增大。2,3,4,7,8-PeCDF对总的毒性当量贡献最大,占总毒性当量浓度的38.87%。六个采样点中有三个地点二噁同系物分布显示了"源"的特征,而另外三个地点则显示了"汇"的特征。成人的PCDD/Fs暴露量为0.0023～0.047 pg I-TEQ/kg.day;儿童PCDD/Fs暴露量为0.0052～0.11 pg I-TEQ/kg.day。结论:深圳市大气样品中二噁浓度低于国内一些城市研究水平,而高于日本、欧美国家的研究水平。     

Development of a new automated clean-up system for the simultaneous analysis of polychlorinated dibenzo-p-dioxins (PCDDs), dibenzofurans (PCDFs) and 'dioxin-like' polychlorinated biphenyls (dl-PCB) in flue gas emissions by GPC-SPE

A comprehensive clean-up method for quantitative analysis of polychlorinated biphenyls (PCBs) and polychlorinated dibenzo-p-dioxins and dibenzo-furans (PCDD/Fs) in one single extract of environmental samples was developed. Since the chemical nature and toxicity of planar PCBs are similar to those of PCDD/Fs, dioxin-like PCBs and PCDD/Fs are often surveyed together in their exposure assessments. The development of a method for the simultaneous analysis of PCBs and PCDD/Fs in environmental samples is invaluable. The automated clean-up system evaluated in this work consists of three additional steps after traditional extraction: the chromatography on gel permeation (GPC), the concentration of the solvent through the use of an in-line evaporation module and the further purification and separation of PCDDs/Fs and dl-PCBs on an alumina cartridge in the 'SPE module'. In this work, three fly ash samples from an interlaboratory study with different PCDD/F and PCB levels were Soxhlet-extracted and then cleaned up using an automated system. PCDD/Fs and PCBs were determined using isotope dilution and high resolution gas chromatography/high resolution mass spectrometry. The determined values of 17 PCDD/Fs were consistent with the certified values and the relative standard deviations (RSDs) of the determined values were less than 20%. The recoveries of (13)C labeled PCDD/Fs and planar PCBs, and their RSDs were within the ranges specified in EPA1613 and 1668a methods, respectively. An accurate and reliable method was successfully developed and can be used in the simultaneous analysis of PCDD/Fs and planar PCBs in environmental samples.     

杭州城区环境空气中二口恶英浓度状况研究

依据2009年7月至2012年2月连续3年对杭州城区环境空气中二英（PCDD/Fs）采样分析结果得知，杭州城区环境空气中二英毒性当量质量浓度变化范围为0.13～0.55 pg TEQ/m³，均值为0.34 pg TEQ/m³。城区环境空气中二英浓度季节变化不显著，夏季略低于冬季；城区范围内不同功能区之间二英浓度差别不显著；连续3年监测结果未显现二英年度变化趋势。沙尘暴天气环境空气中二英浓度显著增高，日常天气和烟花爆竹集中燃放天气环境空气中二英形态分布存在明显区别，烟花爆竹集中燃放期间八氯代二苯并-对-二英（OCDD）占总质量浓度比例显著提高。利用IBM SPSS Statistics 19.0统计软件对24个监测结果聚类分析发现，杭州城区环境空气中二英的同类物分布具有明显的“源”分布特征。     

Mussel watch program for organic contaminants along the Korean coast, 2001–2007

The level and extent of organic contaminants along the Korean coast were estimated through the mussel watch program, established in 2001. Mussels and oysters were collected at 20 sites along the Korean coast in 2001 and at 25 sites from 2002 to 2007. The mussel tissues were analyzed for PCBs, organochlorine presticides, PAHs, BTs, and PCDD/Fs. PCBs, PAHs, BTs, and PCDD/Fs were ubiquitous contaminants along the Korean coast, showing mean detection frequencies of more than 95% over 7 years. The concentrations of organic contaminants in mussels along the Korean coast were relatively low or moderate compared with foreign studies. Concentrations of DDTs, PCBs, and PCDD/Fs were below the action or maximum levels for humans established by USFDA and EU. Elevated concentrations above the 85th percentile were found for PCBs, PAHs, BTs, and PCDD/Fs at sites near industrial complexes or big harbors, for HCHs at sites near non-industrial complexes, and for DDTs at sites near both non-industrial and industrial complexes. Using two nonparametric tests to assess temporal trends, the Spearman test revealed that BTs and PCDD/Fs had significant decreasing trends at four sites (Gwangyang Bay, Cheonsu Bay, Garorym Bay, and the Incheon coast) and at six sites (Hupo coast, Guryongpo coast, eastern part of Geojedo, Gunsan coast, Garorym Bay, and Asan Bay), respectively.     

Seasonal variation of polycyclic aromatic hydrocarbons in soil and air of Dalian areas, China: an assessment of soil-air exchange

The seasonal variations of concentrations of PAHs in the soil and the air were measured in urban and rural region of Dalian, China in 2007. In soil, mean concentrations of all PAHs in summer were larger than those in winter, whereas the concentrations of heavier weight PAHs in winter were larger than those in summer. Winter/summer concentration ratios for individual PAHs (R(W/S)) increased with the increase of molecular weight of PAHs in soil, indicating that PAHs with high molecular weight were more easily deposited to soil in winter than summer. In air, mean concentrations of all PAHs in winter were larger than those in summer. In comparison with the R(W/S) in soil, all the values of R(W/S) in air were larger than one indicating that the entire individual PAH concentrations in winter were larger than those in summer. The average concentration composition for each PAH compound in soil and air samples was determined and the seasonal change of PAH profile was very small. It was suggested that PAHs in soils and air had the same or similar sources both in winter and summer. The approach to the soil-air equilibrium was assessed by calculating fugacity quotients between soil and air using the soil and air concentrations. The calculated soil-air fugacity quotients indicated that soil acted as a secondary source to the atmosphere for all lighter weight PAHs (two-three rings) and it will continue to be a sink for heavier weight PAHs (five-six rings) in the Dalian environment, both in winter and summer. Medium weight PAHs (four-five rings) were close to the soil-air equilibrium and the tendency shifted between soil and air when season or function region changed. The fugacity quotients of PAHs in summer (mean temperature 298 K) were larger than those in winter (mean temperature 273 K), indicating a higher tendency in summer than winter for PAHs to move from soil to air. The variation of ambient conditions such as temperature, rainfall, etc. can influence the movement of PAHs between soil and air. Most of the fugacity quotients of PAHs for the urban sites were larger than that for the rural site both in winter and summer. This phenomenon may be related with that the temperatures in urban sites were higher than those in the rural site because of the urban heat island effect.     

Study of air-soil exchange of polycyclic aromatic hydrocarbons (PAHs) in the north-central part of India--a semi arid region

Soil is the major environmental reservoir of organic compounds and soil-air exchange is a key process in governing the environmental fate of these compounds on a regional and global scale. Samples of air and soil were collected to study the levels of PAHs in the air and soil of the Agra region. Concentrations of PAH measured at four locations in the city of Agra, covers industrial, residential, roadside and agricultural areas. Samples were extracted with hexane by ultrasonic agitation. Extracts were then fractioned on a silica-gel column and the aromatic fraction was analysed by GC-MS. The mean concentration of the total PAH (T-PAH) in the air of Agra was 24.95, 17.95 and 14.25 ng m(-3), during winter, monsoon and summer respectively. The average concentration of T-PAH in the soil of Agra was 12.50, 8.25 and 6.44 μg g(-1) in winter, monsoon and summer seasons respectively. The aim of this study was to investigate the rate of approach to equilibrium partitioning of PAHs between air and soil compartments and to determine the direction of net flux of the studied PAH between air and soil. Calculated soil-air fugacity quotients indicate that the soil may now be a source of some lighter weight PAHs to the atmosphere, whereas it appears to be still acting as a long-term sink for the heavier weight PAHs to some extent in this region.     

Receptor modeling for analyzing PCDD/F and dioxin-like PCB sources in Hong Kong

A total of 96 ambient air samples were collected from January 2004 to December 2004 for the investigation of dioxins (polychlorinated dibenzo-para-dioxins and polychlorinated dibenzofurans [PCDD/Fs]) and dioxin-like profile for polychlorinated biphenyls (PCBs) in the atmosphere of Hong Kong. Two-day back-trajectories were obtained using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model from National Oceanic and Atmospheric Administration (NOAA) Air Resources Laboratory. Receptor models – potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) – were built based on the measured PCDD/Fs and dioxin-like PCBs total toxic equivalent (TEQ) concentrations. Both models were modified in this study so as to integrate the information obtained from three sampling sites in Hong Kong. The PSCF modeling resolved two main PCDD/F and dioxin-like PCB polluting paths from Mainland China. In line with previous studies, the northerly path around the Pearl River Delta might be one of the pollution sources of Hong Kong air. On the other hand, the receptor models also indicated another potential northeasterly source from Yangtze River Delta, which was seldom mentioned as the source region of Hong Kong air. Results from the CWT modeling suggested that the most toxic air mass affecting Hong Kong is probably attributable to the northeast path rather than the north path.