Modeling the atmospheric transport and outflow of polycyclic aromatic hydrocarbons emitted from China

Modeling the atmospheric transport and outflow of polycyclic aromatic hydrocarbons emitted from China
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对中国排放的多环芳烃的大气传输和流出进行建模

DOI:
10.1016/j.atmosenv.2011.03.006
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发表时间:
2011-06
影响因子:
5
通讯作者:
Shen, Huizhong
Shen, Huizhong
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Zhang, Yanxu;Tao, Shu;Ma, Jianmin;Shen, Huizhong

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2003年,基于平方公里分辨率的排放清单,将欧拉大气迁移模型CanMETOP(加拿大有机氯农药环境迁移模型)应用于中国多环芳烃(PAHs)的大气迁移和流出。还考虑了与 OH 自由基的反应、考虑总气溶胶表面积吸附的气体/颗粒分配以及多环芳烃的动态土壤/海洋-空气交换。结果表明,大气中PAH浓度水平的空间分布很大程度上受排放和气象条件的控制。由于山西、贵州、华北平原、四川盆地和重庆都市圈的排放密度较高,预计这些地区的浓度水平将会升高。在中国近海和西太平洋的环境中也模拟了高浓度。该模型还预测行星边界层的垂直剖面略有下降(低于~1公里),但自由大气中的浓度下降~2个数量级。西风带、东亚季风和当地地形强迫被认为是影响中国多环芳烃迁移模式的关键因素。 2003年,美国环境保护局优先控制清单上所列的16种多环芳烃母体中约有3800吨被运出中国,其中约80%是通过东部边境运输的。流出量集中在 30°N 附近,这表明与发射密度峰值的位置略有差异。流出羽流的中心位于东经 120° 约 1 公里的高度,在东经 130° 和 140° 分别上升到 3.5 公里和 5 公里。流出通量也存在 5-6 倍的季节性变化,春季和冬季运输通量大大增加。
An Euler atmospheric transport model CanMETOP (Canadian Model for Environmental Transport of Organochlorine Pesticides) was applied to the atmospheric transport and outflow of polycyclic aromatic hydrocarbons (PAHs) in China in 2003 based on a square kilometer resolution emission inventory. The reaction with OH radical, gas/particle partition by considering the adsorption onto total aerosol surface area, and dynamic soil/ocean–air exchange of PAHs were also considered. The results show that the spatial distribution of PAH concentration levels in the atmosphere is greatly controlled by emission and meteorological conditions. Elevated concentration levels are predicted in Shanxi, Guizhou, North China Plain, Sichuan Basin and Chongqing metropolitan areas due to the high emission densities at those locations. High concentrations are also modeled in environments offshore of China and in the western Pacific Ocean. The model also predicts a slightly decreasing vertical profile in the planetary boundary layer (lower than ∼1 km), but concentration decreases ∼2 orders of magnitude in the free atmosphere. The Westerlies as well as the East Asian Monsoon and local topographical forcings are identified as key factors influencing the transport pattern of PAHs in China. In 2003, ∼3800°tons of the sixteen parent PAHs listed on USEPA priority control list were transported out of China with about 80% transported through the eastern boundary. The outflow concentrates near 30°N, signifying a slight discrepancy from the position of emission density peaks. The center of the outflow plume is located at a height of ∼1 km at 120°E, and climbs to 3.5 km and 5 km at 130°E and 140°E, respectively. A seasonal variation of 5–6 fold is also found for the outflow flux with greatly elevated transport flux in spring and winter.
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