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新泽西州卡姆登市个人及周围环境中的空气有毒物质暴露情况。

Personal and ambient exposures to air toxics in Camden, New Jersey.

作者信息

Lioy Paul J, Fan Zhihua, Zhang Junfeng, Georgopoulos Panos, Wang Sheng-Wei, Ohman-Strickland Pamela, Wu Xiangmei, Zhu Xianlei, Harrington Jason, Tang Xiaogang, Meng Qingyu, Jung Kyung Hwa, Kwon Jaymin, Hernandez Marta, Bonnano Linda, Held Joann, Neal John

机构信息

Environmental and Occupational Health Sciences Institute, Robert Wood Johnson Medical School, Piscataway, New Jersey 08854, USA.

出版信息

Res Rep Health Eff Inst. 2011 Aug(160):3-127; discussion 129-51.

Abstract

Personal exposures and ambient concentrations of air toxics were characterized in a pollution "hot spot" and an urban reference site, both in Camden, New Jersey. The hot spot was the city's Waterfront South neighborhood; the reference site was a neighborhood, about 1 km to the east, around the intersection of Copewood and Davis streets. Using personal exposure measurements, residential ambient air measurements, statistical analyses, and exposure modeling, we examined the impact of local industrial and mobile pollution sources, particularly diesel trucks, on personal exposures and ambient concentrations in the two neighborhoods. Presented in the report are details of our study design, sample and data collection methods, data- and model-analysis approaches, and results and key findings of the study. In summary, 107 participants were recruited from nonsmoking households, including 54 from Waterfront South and 53 from the Copewood-Davis area. Personal air samples were collected for 24 hr and measured for 32 target compounds--11 volatile organic compounds (VOCs*), four aldehydes, 16 polycyclic aromatic hydrocarbons (PAHs), and particulate matter (PM) with an aerodynamic diameter < or = 2.5 microm (PM2.5). Simultaneously with the personal monitoring, ambient concentrations of the target compounds were measured at two fixed monitoring sites, one each in the Waterfront South and Copewood-Davis neighborhoods. To understand the potential impact of local sources of air toxics on personal exposures caused by temporal (weekdays versus weekend days) and seasonal (summer versus winter) variations in source intensities of the air toxics, four measurements were made of each subject, two in summer and two in winter. Within each season, one measurement was made on a weekday and the other on a weekend day. A baseline questionnaire and a time diary with an activity questionnaire were administered to each participant in order to obtain information that could be used to understand personal exposure to specific air toxics measured during each sampling period. Given the number of emission sources of air toxics in Waterfront South, a spatial variation study consisting of three saturation-sampling campaigns was conducted to characterize the spatial distribution of VOCs and aldehydes in the two neighborhoods. Passive samplers were used to collect VOC and aldehyde samples for 24- and 48-hr sampling periods simultaneously at 22 and 16 grid-based sampling sites in Waterfront South and Copewood-Davis, respectively. Results showed that measured ambient concentrations of some target pollutants (mean +/- standard deviation [SD]), such as PM2.5 (31.3 +/- 12.5 microg/m3), toluene (4.24 +/- 5.23 microg/m3), and benzo[a]pyrene (0.36 +/- 0.45 ng/m3), were significantly higher (P < 0.05) in Waterfront South than in Copewood-Davis, where the concentrations of PM2.5, toluene, and benzo[a]pyrene were 25.3 +/- 11.9 microg/m3, 2.46 +/- 3.19 microg/m3, and 0.21 +/- 0.26 ng/m3, respectively. High concentrations of specific air toxics, such as 60 microg/m3 for toluene and 159 microg/m3 for methyl tert-butyl ether (MTBE), were also found in areas close to local stationary sources in Waterfront South during the saturation-sampling campaigns. Greater spatial variation in benzene, toluene, ethylbenzene, and xylenes (known collectively as BTEX) as well as of MTBE was observed in Waterfront South than in Copewood-Davis during days with low wind speed. These observations indicated the significant impact of local emission sources of these pollutants and possibly of other pollutants emitted by individual source types on air pollution in Waterfront South. (Waterfront South is a known hot spot for these pollutants.) There were no significant differences between Waterfront South and Copewood-Davis in mean concentrations of benzene or MTBE, although some stationary sources of the two compounds have been reported in Waterfront South. Further, a good correlation (R > 0.6) was found between benzene and MTBE in both locations. These results suggest that automobile exhausts were the main contributors to benzene and MTBE air pollution in both neighborhoods. Formaldehyde and acetaldehyde concentrations were found to be high in both neighborhoods. Mean (+/- SD) concentrations of formaldehyde were 20.2 +/- 19.5 microg/m3 in Waterfront South and 24.8 +/- 20.8 microg/m3 in Copewood-Davis. A similar trend was observed for the two compounds during the saturation-sampling campaigns. The results indicate that mobile sources (i.e., diesel trucks) had a large impact on formaldehyde and acetaldehyde concentrations in both neighborhoods and that both are aldehyde hot spots. The study also showed that PM2.5, aldehydes, BTEX, and MTBE concentrations in both Waterfront South and Copewood-Davis were higher than ambient background concentrations in New Jersey and than national average concentrations, indicating that both neighborhoods are in fact hot spots for these pollutants. Higher concentrations were observed on weekdays than on weekend days for several compounds, including toluene, ethylbenzene, and xylenes (known collectively as TEX) as well as PAHs and PM2.5. These observations showed the impact on ambient air pollution of higher traffic volumes and more active industrial and commercial operations in the study areas on weekdays. Seasonal variations differed by species. Concentrations of TEX, for example, were found to be higher in winter than in summer in both locations, possibly because of higher emission rates from automobiles and reduced photochemical reactivity in winter. In contrast, concentrations of MTBE were found to be significantly higher in summer than in winter in both locations, possibly because of higher evaporation rates from gasoline in summer. Similarly, concentrations of heavier PAHs, such as benzo[a]pyrene, were found to be higher in winter in both locations, possibly because of higher emission rates from mobile sources, the use of home heating, and the reduced photochemical reactivity of benzo[a]pyrene in winter. In contrast, concentrations of lighter PAHs were found to be higher in summer in both locations, possibly because of volatilization of these compounds from various surfaces in summer. In addition, higher concentrations of formaldehyde were observed in summer than in winter, possibly because of significant contributions from photochemical reactions to formaldehyde air pollution in summer. Personal concentrations of toluene (25.4 +/- 13.5 microg/m3) and acrolein (1.78 +/- 3.7 microg/m3) in Waterfront South were found to be higher than those in the Copewood-Davis neighborhood (13.1 +/- 15.3 microg/m3 for toluene and 1.27 +/- 2.36 microg/m3 for acrolein). However, personal concentrations for most of the other compounds measured in Waterfront South were found to be similar to or lower than those than in Copewood-Davis. (For example, mean +/- SD concentrations were 4.58 +/- 17.3 microg/m3 for benzene, 4.06 +/- 5.32 microg/m3 for MTBE, 16.8 +/- 15.5 microg/m3 for formaldehyde, and 0.40 +/- 0.94 ng/m3 for benzo[a]pyrene in Waterfront South and 9.19 +/- 34.0 microg/m3 for benzene, 6.22 +/- 19.0 microg/m3 for MTBE, 16.0 +/- 16.7 microg/m3 for formaldehyde, and 0.42 +/- 1.08 ng/m3 for benzo[a]pyrene in Copewood-Davis.) This was probably because many of the target compounds had both outdoor and indoor sources. The higher personal concentrations of these compounds in Copewood-Davis might have resulted in part from higher exposure to environmental tobacco smoke (ETS) of subjects from Copewood-Davis. The Spearman correlation coefficient (R) was found to be high for pollutants with significant outdoor sources. The R's for MTBE and carbon tetrachloride, for example, were > 0.65 in both Waterfront South and Copewood-Davis. The R's were moderate or low (0.3-0.6) for compounds with both outdoor and indoor sources, such as BTEX and formaldehyde. A weaker association (R < 0.5) was found for compounds with significant indoor sources, such as BTEX, formaldehyde, PAHs, and PM2.5. The correlations between personal and ambient concentrations of MTBE and BTEX were found to be stronger in Waterfront South than in Copewood-Davis, reflecting the significant impact of local air pollution sources on personal exposure to these pollutants in Waterfront South. Emission-based ambient concentrations of benzene, toluene, and formaldehyde and contributions of ambient exposure to personal concentrations of these three compounds were modeled using atmospheric dispersion modeling and Individual Based Exposure Modeling (IBEM) software, respectively, which were coupled for analysis in the Modeling Environment for Total Risk (MENTOR) system. The compounds were associated with the three types of dominant sources in the two neighborhoods: industrial sources (toluene), exhaust from gasoline-powered motor vehicles (benzene), and exhaust from diesel-powered motor vehicles (formaldehyde). Subsequently, both the calculated and measured ambient concentrations of each of the three compounds were separately combined with the time diaries and activity questionnaires completed by the subjects as inputs to IBEM-MENTOR for estimating personal exposures from ambient sources. Modeled ambient concentrations of benzene and toluene were generally in agreement with the measured ambient concentrations within a factor of two, but the values were underestimated at the high-end percentiles. The major local (neighborhood) contributors to ambient benzene concentrations were from mobile sources in the study areas; both mobile and stationary (point and area) sources contributed to the ambient toluene concentrations. This finding can be used as guidance for developing better emission inventories to characterize, through modeling, the ambient concentrations of air toxics in the study areas. (ABSTRACT TRUNCATED)

摘要

在新泽西州卡姆登市的一个污染“热点地区”和一个城市参考地点,对空气有毒物质的个人暴露量和环境浓度进行了表征。热点地区是该市的滨海南区;参考地点是位于以东约1公里处、科普伍德街和戴维斯街交叉路口周围的一个社区。我们通过个人暴露测量、住宅环境空气测量、统计分析和暴露建模,研究了当地工业和移动污染源,特别是柴油卡车,对这两个社区个人暴露量和环境浓度的影响。报告中介绍了我们的研究设计、样本和数据收集方法、数据及模型分析方法,以及研究结果和主要发现。总之,我们从非吸烟家庭招募了107名参与者,其中54名来自滨海南区,53名来自科普伍德 - 戴维斯地区。采集了24小时的个人空气样本,测量了32种目标化合物——11种挥发性有机化合物(VOCs*)、4种醛类、16种多环芳烃(PAHs)以及空气动力学直径小于或等于2.5微米的颗粒物(PM2.5)。在进行个人监测的同时,在两个固定监测点测量了目标化合物的环境浓度,滨海南区和科普伍德 - 戴维斯社区各有一个监测点。为了解空气有毒物质的当地来源因时间(工作日与周末)和季节(夏季与冬季)变化导致的源强变化对个人暴露的潜在影响,对每个受试者进行了四次测量,夏季两次,冬季两次。在每个季节内,一次测量在工作日进行,另一次在周末进行。向每位参与者发放了一份基线调查问卷以及一份带有活动问卷的时间日志,以获取可用于了解在每个采样期间个人对特定空气有毒物质暴露情况的信息。鉴于滨海南区空气有毒物质排放源的数量,开展了一项由三次饱和采样活动组成的空间变化研究,以表征这两个社区中VOCs和醛类的空间分布。分别在滨海南区和科普伍德 - 戴维斯的22个和16个基于网格划分的采样点,使用被动采样器在24小时和48小时的采样期内同时采集VOC和醛类样本。结果显示,滨海南区某些目标污染物的实测环境浓度(平均值±标准差[SD]),如PM(31.3±12.5微克/立方米)、甲苯(4.24±5.23微克/立方米)和苯并[a]芘(0.36±0.45纳克/立方米),显著高于(P<0.05)科普伍德 - 戴维斯地区,该地区PM2.5、甲苯和苯并[a]芘的浓度分别为25.3±11.9微克/立方米、2.46±3.19微克/立方米和0.21±0.26纳克/立方米。在饱和采样活动期间,在滨海南区靠近当地固定源的区域还发现了高浓度的特定空气有毒物质,如甲苯浓度达60微克/立方米,甲基叔丁基醚(MTBE)浓度达159微克/立方米。在风速较低的日子里,滨海南区苯、甲苯、乙苯和二甲苯(统称为BTEX)以及MTBE的空间变化比科普伍德 - 戴维斯地区更大。这些观察结果表明这些污染物的当地排放源以及可能由个别源类型排放的其他污染物对滨海南区空气污染有显著影响。(滨海南区是这些污染物的已知热点地区。)尽管在滨海南区已报告有这两种化合物的一些固定源,但滨海南区和科普伍德 - 戴维斯地区苯或MTBE的平均浓度没有显著差异。此外,在两个地点苯和MTBE之间都发现了良好的相关性(R>0.6)。这些结果表明汽车尾气是这两个社区苯和MTBE空气污染的主要来源。在两个社区都发现甲醛和乙醛浓度较高。滨海南区甲醛的平均(±SD)浓度为20.2±19.5微克/立方米,科普伍德 - 戴维斯地区为24.8±20.8微克/立方米。在饱和采样活动期间,这两种化合物也观察到类似趋势。结果表明移动源(即柴油卡车)对两个社区的甲醛和乙醛浓度有很大影响且这两个社区都是醛类热点地区。该研究还表明,滨海南区和科普伍德 - 戴维斯地区的PM2.5、醛类、BTEX和MTBE浓度均高于新泽西州的环境背景浓度以及全国平均浓度,这表明这两个社区实际上都是这些污染物的热点地区。包括甲苯、乙苯和二甲苯(统称为TEX)以及PAHs和PM2.5在内的几种化合物在工作日的浓度高于周末。这些观察结果表明工作日研究区域内较高的交通流量以及更活跃的工商业运营对环境空气污染的影响。不同物种的季节变化有所不同。例如,在两个地点TEX的浓度冬季均高于夏季,这可能是由于冬季汽车排放率较高且光化学反应性降低。相反,在两个地点MTBE的浓度夏季均显著高于冬季,这可能是由于夏季汽油蒸发率较高。同样,在两个地点较重的PAHs如苯并[a]芘的浓度冬季均较高,这可能是由于移动源排放率较高、使用家庭取暖以及冬季苯并[a]芘光化学反应性降低。相反,较轻的PAHs浓度在两个地点夏季均较高,这可能是由于这些化合物在夏季从各种表面挥发。此外,夏季甲醛浓度高于冬季,这可能是由于光化学反应对夏季甲醛空气污染有显著贡献。滨海南区甲苯(25.4±13.5微克/立方米)和丙烯醛(1.78±3.7微克/立方米)的个人浓度高于科普伍德 - 戴维斯社区(甲苯为13.1±15.3微克/立方米,丙烯醛为1.27±2.36微克/立方米)。然而,在滨海南区测量的大多数其他化合物的个人浓度与科普伍德 - 戴维斯地区相似或更低。(例如,滨海南区苯的平均(±SD)浓度为4.58±17.3微克/立方米,MTBE为4.06±5.32微克/立方米,甲醛为16.8±15.5微克/立方米,苯并[a]芘为0.40±0.94纳克/立方米;科普伍德 - 戴维斯地区苯为9.19±34.0微克/立方米,MTBE为6.22±19.0微克/立方米,甲醛为16.0±16.7微克/立方米,苯并[a]芘为0.42±1.08纳克/立方米。)这可能是因为许多目标化合物既有室外来源也有室内来源。科普伍德 - 戴维斯地区这些化合物较高的个人浓度可能部分是由于该地区受试者对环境烟草烟雾(ETS)的暴露较高。对于具有显著室外来源的污染物,斯皮尔曼相关系数(R)较高。例如,滨海南区和科普伍德 - 戴维斯地区MTBE和四氯化碳的R均>0.65。对于既有室外来源又有室内来源地化合物如BTEX和甲醛,R为中等或较低(0.3 - 0.6)。对于具有显著室内来源的化合物如BTEX、甲醛、PAHs和PM2.5,关联较弱(R<0.5)。滨海南区MTBE和BTEX的个人浓度与环境浓度之间的相关性比科普伍德 - 戴维斯地区更强,这反映了当地空气污染源对滨海南区个人对这些污染物暴露的显著影响。分别使用大气扩散模型和基于个体的暴露建模(IBEM)软件对基于排放的苯、甲苯和甲醛环境浓度以及环境暴露对这三种化合物个人浓度的贡献进行建模,并在总风险建模环境(MENTOR)系统中进行耦合分析。这些化合物与两个社区的三种主要源类型相关:工业源(甲苯)、汽油动力机动车尾气(苯)和柴油动力机动车尾气(甲醛)。随后,将这三种化合物各自计算得到的和实测的环境浓度分别与受试者填写的时间日志和活动问卷相结合,作为输入到IBEM - MENTOR中以估计来自环境源的个人暴露量。苯和甲苯的模拟环境浓度与实测环境浓度总体上在两倍因子范围内一致,但在高端百分位数处数值被低估。研究区域内环境苯浓度的主要本地(社区)贡献者来自移动源;移动源和固定(点源和面源)源都对环境甲苯浓度有贡献。这一发现可作为指导,用于制定更好的排放清单,通过建模来表征研究区域内空气有毒物质的环境浓度。(摘要截断)

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