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Scavenging ratios of polycyclic aromatic compounds in rain and snow in the Athabasca oil sands region

机译:高雪地油砂区域雨雪中多环芳烃的清除比例

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The Athabasca oil sands industry in northern Alberta, Canada, is a possible source of polycyclic aromatic compounds (PACs). Monitored PACs, including polycyclic aromatic hydrocarbons (PAHs), alkylated PAHs, and dibenzothiophenes (DBTs), in precipitation and in air at three near-source sites in the Fort MacKay and Fort McMurray area during January 2011 to May 2012, were used to generate a database of scavenging ratios (Wt) for PACs scavenged by both snow and rain. Higher concentrations in precipitation and air were observed for alkylated PAHs and DBTs compared to the other PACs. The sums of the median precipitation concentrations over the period of data analyzed were 0.48 μ g L?1 for the 18 PAHs, 3.38 μ g L?1 for the 20 alkylated PAHs, and 0.94 μ g L?1 for the 5 DBTs. The sums of the median air concentrations for parent PAHs, alkylated PAHs, and DBTs were 8.37, 67.26, and 11.83 ng m?3, respectively. Median Wt over the measurement period were 6100 1.1 106 from snow scavenging and 350 2.3 105 from rain scavenging depending on the PAC species. Median Wt for parent PAHs were within the range of those observed at other urban and suburban locations, but Wt for acenaphthylene in snow samples were 2–7 times higher compared to other urban and suburban locations. Wt for some individual snow and rain samples exceeded literature values by a factor of 10. Wt for benzo(a)pyrene, dibenz(a,h)anthracene, and benzo(g,h,i)perylene in snow samples had reached 107, which is the maximum for PAH snow scavenging ratios reported in the literature. From the analysis of data subsets, Wt for particulate-phase dominant PACs were 14–20 times greater than gas-phase dominant PACs in snow samples and 7–20 times greater than gas-phase dominant PACs in rain samples. Wt from snow scavenging were ~ 9 times greater than from rain scavenging for particulate-phase dominant PACs and 4–9.6 times greater than from rain scavenging for gas-phase dominant PACs. Gas-particle fractions of each PAC, particle size distributions of particulate-phase dominant PACs, and the Henry's law constant of gas-phase dominant PACs explained, to a large extent, the different Wt values among the different PACs and precipitation types. The trend in Wt with increasing alkyl substitutions may be attributed to their physico-chemical properties, such as octanol–air and particle partition coefficients and subcooled vapor pressure, which increases gas-particle partitioning and, subsequently, the particulate mass fraction. This study verified findings from a previous study of Wang et al. (2014) that suggested that snow scavenging is more efficient than rain scavenging of particles for equivalent precipitation amounts, and also provided new knowledge of the scavenging of gas-phase PACs and alkylated PACs by snow and rain.
机译:加拿大艾伯塔北部的阿萨巴斯卡油砂产业是多环芳烃(PACS)的可能源。在2011年1月至2012年1月至2012年5月,在2012年1月至2012年5月,在2011年1月至2012年5月,在2011年至2012年5月的三个近源地区,包括多环芳烃(PAH),烷基化的PAHs和二苯脲蛋白(DBTS),沉淀和空气中的溶解型芳烃和二苯并噻吩(DBT),用于产生雪和雨水清除的PACS的清除比率(WT)数据库。与其他PACS相比,观察到烷基化的PAHS和DBTs的沉淀和空气中的较高浓度。分析的数据期间的中值沉淀浓度的总和为18pah的0.48μgl= 1,对于20个烷基化的pAh,3.38μgl≥1,为5 dbts为0.94μgl= 1。亲本PAH,烷基化PAH和DBT的中位空气浓度的总和分别为8.37,67.26和11.83ngm≤3。测量期间的中位数WT为6100 1.1 106,雪清扫管和350 2.3 105根据PAC物种,从雨水清除。对于父母PAH的中位数WT在其他城市和郊区地区观察到的那些范围内,但与其他城市和郊区的地点相比,雪样上的加法纳西萘二甲苯比为2-7倍。对于一些单独的雪和雨水样本超过文学值10.苯并(a)芘,二苯苯(a,h)蒽和苯并(g,h,i)鲍尔在雪样中达到107倍,这是文献中报告的PAH雪扫描比率最高。根据数据子集的分析,对于颗粒相占优势PAC的WT比雪样中的气相显性PACs大14-20倍,比雨水样本中的气相显性PACs大7-20倍。来自雪清除的WT比雨水清除颗粒相位优势PACs的〜9倍,比从雨水淘汰的气相占优势PACS的雨水扫描4-9.6倍。每种PAC的气体颗粒粒径,颗粒阶段优势PACs的粒度分布,以及亨利的气相显性PAC的常数在很大程度上解释了不同PACS和沉淀类型之间的不同WT值。随着烷基取代的增加,WT的趋势可以归因于它们的物理化学性质,例如辛醇 - 空气和颗粒分配系数和脱池蒸气压,这增加了气体颗粒分配,随后,颗粒质量级分。这项研究来自王等人的先前研究的认证结果。 (2014年)建议雪清扫性比雨清除粒子的雨量较高,并为雪和雨水进行了气相PACS和烷基化的PACS的新知识。

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