北京市大气颗粒物中多环芳烃(PAHs)污染特征

对北京市2003-09～2004-07的10个月空气中的TSP样品进行了连续采样,周期为1次/周.分析了15种3～7环的PAHs,其中以4～5环为主.∑PAHs浓度及BaP的最大值分别达到705 ng/m³和52 ng/m³;春夏秋冬4季∑PAHs的平均浓度分别为46 ng/m³,16 ng/m³,52 ng/m³,268 ng/m³;BaP的4季平均浓度分别为2.8ng/m³,0.23 ng/m³,3.3 ng/m³,16ng/m³;采暖期∑PAHs平均浓度为非采暖期的9.5倍.在所分析的3种气象条件中,降水能够明显降低PAHs的浓度;非采暖期的PAHs浓度随温度的升高而降低,采暖期的浓度与温度没有明显的相关性;采暖期风速水平的增加会导致PAHs浓度的下降,而非采暖期不同环数的PAHs和风速水平的关系各异,3环的PAHs浓度随风速水平增加而增加,4、5环的PAHs浓度变化不大,6、7环PAHs随风速水平的增加而浓度下降.     

利用SPMD技术监测珠江三角洲大气中多环芳烃

利用半渗透膜被动采样装置(SPMD),对珠江三角洲地区大气中多环芳烃进行了分季度为期一年的监测,同时在广州(GZ01站)用大流量采样器进行主动采样分析.结果表明,SPMD主要采集大气气态多环芳烃,其富集速率Rs受温度影响显著,低温更有利于SPMD对有机物的渗透富集.大气气态PAHs浓度季节差异明显,各季度平均值分别为286.0ng/m³(4～6月),322.0ng/m³(7～9月),216.4ng/m³(10～12月)和153.3ng/m³(1～3月),温度是影响气态PAHs含量高低的主因素.该区域内,污染程度呈南北低、中间高.污染源主要来自于机动车尾气的排放.     

广州市大气中多环芳烃分布特征、季节变化及其影响因素

对广州市大气中气态和颗粒态多环芳烃(PAHs)进行了连续一年的采样观测.结果表明,气态和颗粒态样品中PAHs的平均浓度值分别为312.9 ng/m³ 和 23.7 ng/m³,即多环芳烃主要存在于气相中,占大气总PAHs年平均的92.5%,且在夏季的比重要高于冬季.所检出的的气态多环芳烃以芴、菲、蒽等低环数化合物为主,其中菲占了总含量的60%以上;颗粒态多环芳烃则以高环数的化合物为主,各化合物所占的比重相当,其相对浓度无显著差别.气态多环芳烃在夏季达到高值,冬季降为低值;而颗粒态与其相反,夏季低值,冬季达到高值.在所测定的气象条件中,温度在影响气态多环芳烃浓度变化的因素中占了绝对优势,其次为风速,其它气象因素未观测到有较明显的影响作用;对颗粒态多环芳烃来说,则无绝对的影响因素,温度、风速和湿度同为重要影响因素,但随着分子量的增加,各因素的影响大小顺序略有不同.     

北京市民居室内气态PAHs浓度及其影响因素

利用自行改进的被动采样装置收集并测定北京城、近郊区38个家庭在供暖期和非供暖期室内空气中7种气态多环芳烃(PAHs)的浓度和组分谱,并探讨影响室内气态PAHs浓度和组分谱的主要影响因素.分析数据表明,北京城、近郊区民居室内的气态PAHs以2环和3环组分为主,7种气态PAHs组分各自的平均浓度范围为1～40 ng/m³,总平均浓度约为100 ng/m³.供暖期和非供暖期之间7种气态PAHs的总浓度没有表现出显著差异,但苊烯和荧蒽的浓度明显不同.相对于供暖期,非供暖期内2环组分的贡献减少,3、4环组分的比例则增加.根据家庭调查问卷和实测的浓度水平,多因子方差分析的结果显示,北京城、近郊区民居室内气态PAHs的浓度和组分谱的主要影响因素包括吸烟、卫生球使用、居室通风强度、日烹调次数和民居建成时间.     

硅胶腕带被动采集多环芳烃的可行性分析

多环芳烃（polycyclic aromatic hydrocarbons,PAHs）对人体危害巨大,目前关于人体暴露于大气环境PAHs研究主要以主动采样方式开展。硅胶腕带作为一种新的大气被动采样装置,具有体积小、价格低、耐磨耐热、无毒无味等优点,适合人体环境暴露监测。国际上研究刚起步,尚未建立完善的腕带被动采样与主动采样技术之间的定量关系。本研究于2019年秋冬季和2021年冬季在西安市城区,同时开展硅胶腕带被动采样与大气主动采样对低分子量（MW＜203 g·mol^?1）PAHs的对比实验,力求建立两者的联系。2019年和2021年西安冬季大气中低分子量PAHs浓度分别为(52.81±14.76) ng·m^?3和(134.59±39.48) ng·m^?3,与前人研究相当。相对应的腕带浓度为(183.07±40.43) ng·d^?1和(524.99±150.32) ng·d^?1。Pearson相关分析发现：萘、苊烯、1-甲基萘、2-甲基萘、荧蒽以及总PAHs的主、被动采样之间显著相关（P＜0.05）,相关系数均大于0.4,证明硅胶腕带被动采样方法适用于低分子量PAHs的人体暴露监测。     

某焦化厂空气中PAHs的污染现状及健康风险评价

采集并分析了焦化厂不同生产工段环境空气中12种PAHs的浓度.结果表明,在某焦化厂区,12种PAHs浓度之和为11.75～46.66 μg/m³,其中BaP为0.050～1.054 μg/m³;PAHs浓度大小依次为:出焦处＞焦炉顶＞大门口＞熄焦处,焦炉顶和出焦处空气中BaP浓度远高于煤烟和交通干线.用毒性相当因子矫正后的焦化厂区PAHs浓度为0.3875～1.714 μg/m³矫正后的厂区工人口PAHs暴露率为3.100～13.71 μg/m³.     

北京东南郊大气TSP中多环芳烃浓度特征与影响因素

对2005-03～2006-01北京市东南郊3个采样点大气总悬浮颗粒物（TSP）样品进行分析,总结了研究区内TSP以及TSP中16种PAHs的浓度特征和季节变化规律.研究区内16种PAHs浓度总和的范围在0.29～1?184.48 ng/m³之间,均值为239.44 ng/m³;分别用气象参数（温度、风速、气压、相对湿度）和大气API指数（二氧化硫、二氧化氮、PM₁₀）与PAHs浓度进行了偏相关分析,结果表明温度和SO₂的API指数与PAHs浓度相关显著,应用逐步回归方法得到PAHs对气象参数和大气API指数的回归方程,分别为∑16PAHs=572.56-23.18t和∑16PAHs=5.99 SO₂,可以利用温度和SO₂的API指数对PAHs浓度进行估算.     

Fate of PM2.5-bound PAHs in Xiangyang, central China during 2018 Chinese spring festival: Influence of fireworks burning and air-mass transport

Variations of levels, possible source and air mass transmission were investigated for 16 USEPA priority-controlled PAHs in PM_2.5 during 2018 Chinese Spring Festival (CSF) in Xiangyang City, central China which is the North-South pollutant airmass transport channel of China. Totally 37 samples were collected. Mass concentrations of Σ₁₆PAHs for the Pre–CSF day (Pre–CSFD), during the CSF day (CSFD) and after the CSF day (Af–CSFD) are 33.78 ± 17.68 ng/m³, 22.98 ± 6.49 ng/m³, and 8.99 ± 4.44 ng/m³, respectively. High resolution samples showed that Σ₁₆PAHs are higher in the morning (06:00–11:00) or afternoon (11:30–16:30), than those in the evening (17:00–22:00) and at night (22:30–05:30), whereas the result is reversed during the CSFD. Fireworks burning can obviously increase the mass concentration of PAHs. Air mass trajectory indicated that Xiangyang is a sink area of pollutants for northwest and southeast, and the sources of the northeast and southwest. The air mass only can be transmitted out through northeast and southwest. It is effective for improvement of air quality in Wuhan and Hunan to control fireworks emission in Henan and local areas. Fireworks burning was an important source for PAHs during CSFD, biomass, coal combustion, and traffic emission were the main sources of PAHs for Pre–CSFD and Af–CSFD periods. The health risk on the CSFD was higher than the acceptable levels, especially during the intensive fireworks burning, the risk value far exceed 1.0 × 10^?4, controlling burning fireworks is required.     

Yearly variation in characteristics and health risk of polycyclic aromatic hydrocarbons and nitro-PAHs in urban shanghai from 2010–2018

This study encompassed the regular observation of nine polycyclic aromatic hydrocarbons (PAHs) and three nitro-PAHs (NPAHs) in particulate matter (PM) in Shanghai in summer and winter from 2010 to 2018. The results showed that the mean concentrations of ?PAHs in summer decreased by 24.7% in 2013 and 18.1% in 2017 but increased by 10.2% in 2015 compared to the data in 2010. However, the mean concentrations of ?PAHs in winter decreased by 39.7% from 2010 (12.8 ± 4.55 ng/m³) to 2018 (7.72 ± 3.33 ng/m³), and the mean concentrations of 1-nitropyrene in winter decreased by 79.0% from 2010 (42.3 ± 16.1 pg/m³) to 2018 (8.90 ± 2.09 pg/m³). Correlation analysis with meteorological conditions revealed that the PAH and NPAH concentrations were both influenced by ambient temperature. The diagnostic ratios of PAHs and factor analysis showed that they were mainly affected by traffic emissions with some coal and/or biomass combustion. The ratio of 2-nitrofluoranthene to 2-nitropyrene was near 10, which indicated that the OH radical-initiated reaction was the main pathway leading to their secondary formation. Moreover, backward trajectories revealed different air mass routes in each sampling period, indicating a high possibility of source effects from the northern area in winter in addition to local and surrounding influences. Meanwhile, the mean total benzo[a]pyrene-equivalent concentrations in Shanghai in winter decreased by 50.8% from 2010 (1860 ± 645 pg/m³) to 2018 (916 ± 363 pg/m³). These results indicated the positive effects of the various policies and regulations issued by Chinese authorities.     

北京大气PM10中水溶性氯盐的观测研究

氯盐是大气气溶胶中重要水溶性无机盐,对2004年全年北京大气可吸入颗粒中氯盐的变化进行了监测,结果表明北京大气中可溶性氯盐的年均值在(3.1±1.7)μg·m^-3,采暖期平均浓度为(4.6±2.1)μg·m^-3,非采暖期平均浓度为(2.6±1.6)μg·m^-3.最低值出现在5月,为(1.3±0.8)μg·m^-3;最高值出现在12月,为(5.8±5.3)μg·m^-3.日变化在秋冬季多为白天浓度低,晚上浓度高,夏春季多呈现上午高,下午低的特征;季节变化呈现秋冬季高,春夏季低的特点.     

北京市民居室内气态多环芳烃呼吸暴露评价

采用被动采样装置采集并测定北京地区38个家庭采暖期和非采暖期室内空气中的7种气态多环芳烃(PAHs)的含量.结果表明,室内气态PAHs以2、3环组分为主,7种气态PAHs的总平均浓度为100 ng/m3左右.根据实测的PAHs浓度、不同年龄段人群室内平均停留时间及其相应的呼吸速率,计算得到室内成年人(包括老人)对7种气态PAHs的潜在总暴露速率在采暖期和非采暖期分别为66 ng/h和58 ng/h;而未成年人的潜在总暴露速率则分别为56 ng/h和50 ng/h.     

Exposure measurement, risk assessment and source identification for exposure of traffic assistants to particle-bound PAHs in Tianjin, China

To investigate the levels of exposure to particulate-bound polycyclic aromatic hydrocarbon(PAH) and to estimate the risk these levels pose to traffic assistants(TAs) in Tianjin(a megacity in North China), a measurement campaign(33 all-day exposure samples, 25 occupational-exposure samples and 10 indoor samples) was conducted to characterize the TAs' exposure to PAHs, assess the cancer risk and identify the potential sources of exposure. The average total exposure concentration of 14 PAHs was approximately 2871 ± 928 ng/m3(on-duty), and 1622 ± 457 ng/m3(all-day). The indoor PAHs level was 1257 ± 107 ng/m3. After 8000 Monte Carlo simulations, the cancer risk resulting from exposure to PAHs was found to be approximately 1.05 × 10-4. A multivariate analysis was applied to identify the potential sources, and the results showed that, in addition to vehicle exhaust, coal combustion and cooking fumes were also another two important contributors to personal PAH exposure. The diagnostic ratios of PAH compounds agree with the source apportionment results derived from principal component analysis.     

武汉市大气PM2.5中多环芳烃的分布特征及来源

为研究武汉市大气质量状况,在武汉市ID（工业区）、DT（中心城区）、BG（植物园）设3个采样点,连续1 a同步采集了大气中的PM_2.5（细颗粒物）样品,并研究了其中PAHs（多环芳烃）的质量浓度、来源和健康风险.结果表明,武汉市ID、DT、BG采样点的ρ（PAHs）年均值分别为（75.60±28.12）（59.77±22.81）（24.27±9.15）ng/m3,并呈冬季最高、夏季最低的季节性变化趋势.PMF（正定矩阵因子分析）结果显示,ID、DT、BG采样点的PAHs的主要来源分别为燃煤和扬尘（35%和33%）、机动车和扬尘（30%和34%）、机动车和木质燃烧（33%和32%）,在ID和DT采样点,扬尘对大气颗粒物中PAHs的贡献都很大,而燃煤和木质燃烧分别是ID和BG采样点PAHs的重要来源,在3个采样点中,机动车对颗粒物中PAHs贡献都较大,尤其是DT和BG采样点,机动车的贡献都超过30%.利用后向轨迹模型分析采样期间武汉市的气团来源,并结合每天的ρ（PAHs）发现,不同聚类气团对应的ρ（PAHs）差异很小,表明区域传输对武汉市PAHs贡献不大.通过武汉市大气颗粒物中PAHs吸入风险评估发现,武汉市PAHs的吸入风险范围在10-7~10-5之间,ID和DT采样点的部分人群的吸入风险稍高于安全范围（10-6以下）,有潜在的致癌风险.      

Pollution characteristics and health risk assessment of polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarbons during heating season in Beijing

Polycyclic aromatic hydrocarbons(PAHs) and their nitrated derivatives(NPAHs) attract continuous attention due to their outstanding carcinogenicity and mutagenicity. In order to investigate the diurnal variations, sources, formation mechanism, and health risk assessment of them in heating season, particulate matter(PM) were collected in Beijing urban area from December 26, 2017 to January 17, 2018. PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS). ...     

兰州市PM2.5中多环芳烃的污染特征和来源解析

为了明确兰州市PM_2.5中16种多环芳烃（PAHs）的污染特征和来源,采集了兰州市4个季节的PM_2.5样品,运用气相色谱-质谱联用仪（GC-MS）对PAHs的浓度进行了分析,利用正定矩因子分解法（PMF）、聚类分析和潜在源因子分析法（PSCF）对PAHs的来源进行解析.结果表明,兰州市PM_2.5中ρ（PAHs）均值为：冬季［（118±16.2） ng·m^-3］>秋季［（50.8±21.6） ng·m^-3］>春季［（22.2±8.87） ng·m^-3］>夏季［（4.65±1.32） ng·m^-3］.相关性分析表明,兰州市PM_2.5和TPAHs均与温度呈现极显著的负相关性,与气压呈现极显著的正相关性,与风向、风速和相对湿度的相关性较差.各环PAHs在4个季节的占比相似,其中4环和5环的PAHs占比为最大,其次为6环和2~3环.兰州市PM_2.5中PAHs的主要来源在春夏季为工业排放和生物质及天然气燃烧,秋季工业排放占主导地位,冬季主要为燃煤排放,交通排放在4个季节的贡献比较稳定.聚类分析和PSCF计算结果表明,来自蒙古国、新疆东北部和青海等地的气流对兰州市环境空气质量有重要的影响.     

Variations in traffic-related polycyclic aromatic hydrocarbons in PM2.5 in Kanazawa, Japan, after the implementation of a new vehicle emission regulation

A three-year sampling campaign was conducted at a roadside air pollution monitoring station in the urban area of Kanazawa, Japan. Due to a new emission regulation, PAHs levels decreased over the sampling campaign, exhibiting values of 706 ± 413 pg/m³ in 2017, 559 ± 384 pg/m³ in 2018, and 473 ± 234 pg/m³ in 2019. In each year, similar seasonal variations in PAHs levels were observed, with higher levels observed in winter and lower levels in summer. Among the PAHs isomer ratios, we observed that the ratio of benzo[b]fluoranthene (BbF) and benzo[k]fluoranthene (BkF), [BbF]/([BbF] + [BkF]), and the ratio of indeno[1,2,3-cd]pyrene (IDP) and benzo[ghi]perylene (BgPe), [IDP]/([BgPe] + [IDP]), showed stability over the sampling campaign and were less affected by the new emission regulation, seasonal variations, and regional characteristics. When using the combined ratio ranges of 0.66 - 0.80 ([BbF]/([BbF] + [BkF]) and 0.26-0.49 ([IDP]/([BgPe] + [IDP]), traffic emissions were clearly distinguished from other PAHs emission sources. Principal component analysis (PCA) and positive matrix factorization (PMF) were also performed to further analyse the characteristics of traffic-related PAHs. Overall, this study affirmed the effectiveness of the new emission regulation in the reduction of PAHs emissions and provided a combined range for identifying PAHs traffic emission sources.     

Seasonal variation and sources of derivatized phenols in atmospheric fine particulate matter in North China Plain

Qualitative and quantitative analyses of derivatized phenols in Beijing and in Xinglong were performed from 2016 to 2017 using gas chromatography-mass spectrometry.The results showed substantially more severe pollution in Beijing.Of the 14 compounds detected,the total average concentration was 100 ng/m~3 in Beijing,compared with 11.6 ng/m~3 in Xinglong.More specifically,concentration of nitro-aromatic compounds(NACs)(81.9 ng/m~3 in Beijing and 8.49 ng/m3 in Xinglong) was the highest,followed by aromatic acids(14.6 ng/m~3 in Beijing and 2.42 ng/m~3 in Xinglong) and aromatic aldehydes(3.62 ng/m~3 in Beijing and 0.681 ng/m~3 in Xinglong).In terms of seasonal variation,the highest concentrations were found for 4-nitrocatechol in winter in Beijing(79.1±63.9 ng/m~3) and 4-nitrophenol in winter in Xinglong(9.72±8.94 ng/m~3).The analysis also revealed diurnal variations across different seasons.Most compounds presented higher concentrations at night in winter because of the decreased boundary layer height and increased heating intensity.While some presented higher levels during the day,which attributed to the photo-oxidation process for summer and more biomass burning activities for autumn.Higher concentrations appeared in winter and autumn than in spring and summer,which resulted from more coal combustions and adverse meteorological conditions.The significant correlations among NACs indicated similar sources of pollution.Higher correlations presented within each subgroup than those between the subgroups.Good correlations between levoglucosan and nitrophenols,nitrocatechols,nitro salicylic acids,with correlation coefficients(r) of 0.66,0.69 and 0.69,respectively,indicating an important role of biomass burning among primary sources.     

不同类型紫色土土/气界面汞释放通量及其影响因素

运用动力通量箱与RA-915 汞分析仪联用技术,对重庆市3种类型紫色土的土/气界面汞交换通董进行了实地监测.结果显示,不同类型紫色土的土/气界面汞交换通量有一定差异,随着土壤pH值的增加,汞交换通量值增大,酸性紫色土平均通量值为(30.8±23.7)ng·m-2·h-1,中性紫色土为(34.9±25.7)ng·m-2·h-1,石灰性紫色土为(39.0±27.O)ng·m-2·h-1.土/气界面汞交换量受光照、气温、土壤温度和空气相对湿度等因素的影响,汞交换通量与光照、气温和土壤温度呈显著正相关关系,与相对湿度呈显著负相关关系,与大气压不相关.     

Seasonal variation and source apportionment of organic and inorganic compounds in PM2.5 and PM10 particulates in Beijing, China

The distribution and source of the solvent-extractable organic and inorganic components in PM 2.5(aerodynamics equivalent diameter below 2.5 microns),and PM 10(aerodynamics equivalent diameter below 10 microns) fractions of airborne particles were studied weekly from September 2006 to August 2007 in Beijing.The extracted organic and inorganic compounds identified in both particle size ranges consisted of n-alkanes,PAHs(polycyclic aromatic hydrocarbons),fatty acids and water soluble ions.The potential emission sources of these organic compounds were reconciled by combining the values of n-alkane carbon preference index(CPI),%waxC n,selected diagnostic ratios of PAHs and principal component analysis in both size ranges.The mean cumulative concentrations of n-alkanes reached 1128.65ng/m3 in Beijing,74% of which(i.e.,831.7ng/m3) was in the PM 2.5 fraction,PAHs reached 136.45ng/m3(113.44ng/m3 or 83% in PM 2.5),and fatty acids reached 436.99ng/m3(324.41ng/m3 or 74% in PM 2.5),which resulted in overall enrichment in the fine particles.The average concentrations of SO42-,NO3-,and NH4+ were 21.3±15.2,6.1±1.8,12.5±6.1μg/m3 in PM 2.5,and 25.8±15.5,8.9±2.6,16.9±9.5μg/m3 in PM 10,respectively.These three secondary ions primarily existed as ammonium sulfate((NH4)2SO4),ammonium bisulfate(NH4HSO4) and ammonium nitrate(NH4NO3).The characteristic ratios of PAHs revealed that the primary sources of PAHs were coal combustion,followed by gasoline combustion.The ratios of stearic/palmitic acid indicated the major contribution of vehicle emissions to fatty acids in airborne particles.The major alkane sources were biogenic sources and fossil fuel combustion.The major sources of PAHs were vehicular emission and coal combustion.