Prediction of gas/particle partition quotients of Polybrominated Diphenyl Ethers (PBDEs) in north temperate zone air: an empirical approach.
Prediction of gas/particle partition quotients of Polybrominated Diphenyl Ethers (PBDEs) in north temperate zone air: an empirical approach.
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DOI：
10.1016/j.ecoenv.2014.05.028
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发表时间：
2014-10
影响因子：
6.8
通讯作者：
Yi-Fan Li;Hongliang Jia
中科院分区：
文献类型：
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作者：
Yi-Fan Li;Hongliang Jia
气体/颗粒(G/P)分配过程是控制化学物质在大气中传输和归宿的重要因素。基于中国持久性有机污染物土壤与空气监测二期项目(中国-−-II)获得的700多对气相和颗粒相空气样品，在环境温度从22℃到+38℃的60℃宽范围内，研究了中国空气中多溴二苯醚(PBDEs)的G/P分配行为。我们首次推导了基于过冷液体蒸汽压(PL)和基于辛醇空气分配系数(KOA)的模型的斜率和截距随温度变化的经验方程，从而在不假设平衡状态和没有伪影的情况下预测了分配商(Kp)。这些方程已被成功地应用于预测中国等北温带和东格陵兰北极地区空气中多溴二苯醚的KP值，我们的结果与背景、农村、城市和郊区的监测数据吻合得很好，但在电子垃圾地点却不符合，因为这些地点的多溴二苯醚排放是不可预测的。我们的方程预测了在60°C的温度范围内，LogKP−的斜率范围为0.02-0.82，−-−曲线的斜率范围为0.82-0.02，温度范围为60°C-+38°C。我们的新方程与在平衡条件下导出的−-Bidleman方程进行了比较，结果表明，我们的新方程比Harner-Bidleman方程更好地描述了−-Bidleman方程在空气中的G/P分配行为。我们还首次发现，如果环境温度足够低，多溴二苯醚同系物的G/P分配将在颗粒相相对于气相变得饱和。用logKOA建立了多溴二苯醚的平衡状态和非平衡状态的分类标准。该研究为环境科学家监测和模拟空气中多溴二苯醚的G/P分配行为提供了有用的工具。
Gas/particle (G/P) partitioning process is an important factor governing the transport and fate of chemicals in the atmosphere. Based on a large dataset of more than 700 pairs of air samples in gaseous and particulate phases with a wide ambient temperature range of 60 °C from −22 °C to +38 °C obtained from our Chinese POPs Soil and Air Monitoring Program, Phase 2 (China-SAMP-II), we investigated G/P partitioning behavior of polybrominated diphenyl ether (PBDEs) in Chinese air. We derived for the first time empirical equations to predict the values of slopes and intercepts for both subcooled-liquid–vapor-pressure (PL)-based and octanol-air-partition-coefficient (KOA)-based models as functions of temperature, and thus predicted partition quotient (KP) without assuming an equilibrium status and free of artifacts. These equations have been successfully applied to predict the values ofKPfor PBDEs in air of China and other countries in the north temperate zone (NTZ) and also at an Arctic site in East Greenland, and our results matched the monitoring data well at background, rural, urban, and suburban sites, but not at e-waste sites due to the unpredictable PBDE emissions at these sites. Our equations predicted that the ranges of slopes were 0.02–0.82 for logKP−logKOAplots and −0.82 to −0.02 for logKP−logPLplots at temperatures ranged of 60 °C from −22 °C to +38 °C. Our newKOA-based equation was compared with the Harner–Bidleman equation that was derived at a condition of equilibrium, and the results indicated that our new equation has a better performance than the Harner–Bidleman equation in describing G/P partitioning behavior of PBDEs in air as functions of logKOA. We also found for the first time that the G/P partitioning of PBDE congeners would become saturated in the particulate phase respect to the gas phase if the ambient temperature is low enough. A criterion to classify the equilibrium and nonequilibrium status for PBDEs was also established using logKOA. The study presented in this paper provides a useful tool for environmental scientists in both monitoring and modeling research on G/P partitioning behavior for PBDEs in air.