Multimedia fate modeling of PAHs in Dajiuhu, Shennongjia
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摘要: 选择美国环境保护署EPA优控污染物NaP（萘）、Phe（菲）、Fla（荧蒽）、BaA（苯并蒽）、Chr（屈）、Pyr（芘）和BaP（苯并芘）7种多环芳烃（polycyclic aromatic hydrocarbons，简称PAHs）作为研究对象，采用Level Ⅲ逸度模型对神农架大九湖地区PAHs多介质归趋进行了模拟，并利用神龙架大九湖大气、土壤、水体和沉积物中PAHs的实际监测数据对模型进行了验证；同时，将气候因素（温度、降水）对环境介质中PAHs转化的影响整合进模型中，探讨了气候变化对PAHs归趋的影响。结果表明：模型计算值与研究区PAHs监测值吻合良好，说明模型参数的选取合理可靠；不同PAHs的相间迁移通量具有一定差异，2环和3环PAHs则以沉积物向水体、水体向大气迁移为主，表现出由沉积物向水体和大气释放的特点，而4环和5环PAHs以大气向土壤和水体向沉积物迁移为主，体现出由大气向土壤和沉积物沉降的特点；温度与水-气、土-气和水-沉积物界面交换净通量存在明显的正相关关系，降水量与水-气、土-气界面交换净通量呈负相关关系，但与水-沉积物界面交换净通量呈正相关关系。本研究结果表明应重视因气候变化而引起的土壤、水体、沉积物的内源释放所造成的二次污染。
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关键词:
- Level Ⅲ逸度模型 /
- 大九湖 /
- 多环芳烃 /
- 多介质归趋 /
- 温度变化
Abstract: A Level III fugacity model was used to simulate the fate of seven US-EPA priority polycyclic aromatic hydrocarbons (PAHs), including NaP, Phe, Fla, BaA, Chr, Pyr, and BaP, in Dajiuhu, Shennongjia. Monitoring data of PAHs in study areas were used to verify reliability of this model. Meanwhile, the influence of climate factors (i.e., temperature and precipitation) on the transport of PAHs in different environmental media was integrated into the model to discuss the effect of climate change on the transport trend of PAHs in Dajiuhu. The results show that the data from model computation fits with the measured values of PAHs very well. The transfer flux of different PAHs between different phases is totally different. PHAs of ring 2 and ring 3 are dominated by sediments to water, water to air, indicating the characteristics of releasing from sediments to water and air; while PAHs of ring 4 and ring 5 are dominated by from air to soil and from water to sediments, reflecting the characteristics of deposition from air to soil and sediments. A significant positive correlation between temperature and net flux of water-air, soil-air and sediment-water interface was observed. There was a negative correlation between precipitation and net exchange flux at water-air and soil-air interfaces, while a positive correlation between precipitation and sediment-water interfaces. Our results suggested that attentions should be paid to the secondary pollution release from soil, water and sediment caused by climate change.-
Key words:
- Level Ⅲ multimedia fugacity model /
- Dajiuhu /
- PAHs /
- multimedia fate /
- temperature change
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图 6 水-气、土-气、水-沉积物界面PAHs交换净通量随温度变化
Figure 6. Exchange flux of PAHs at the water-air, soil-air, water-sediment interface changing with temperature
图 7 水-气、土-气、水-沉积物界面PAHs交换净通量随降水量的变化
Figure 7. Exchange flux of PAHs at the water-air, soil-air, water-sediment interface changing with precipitation
参数 NaP Phe Fla BaA Chr Pyr BaP 摩尔质量M/(g·mol-1) 128.19 178.23 202.3 228.3 228.3 202.3 252.3 饱和蒸汽压(25℃)/Pa 10.4 0.02 1.05×10-3 1.5×10-5 5.7×10-7 6×10-4 7×10-7 水溶解度(25℃)/(g·m-3) 31 1.1 0.206 0.009 0.002 0.132 0.003 8 lg Kow 3.37 4.57 5.22 5.91 5.61 5.18 6.04 熔点/℃ 80.5 101 166 177 255 156 175 气相中半衰期/h 17 55 170 170 170 170 170 水相中半衰期/h 170 550 1 700 1 700 1 700 1 700 1 700 土壤相中半衰期/h 1 700 5 500 17 000 17 000 17 000 17 000 17 000 沉积物相中半衰期/h 5 500 17 000 55 000 55 000 55 000 55 000 55 000 鱼子相中半衰期/h 170 550 1 700 1 700 1 700 1 700 1 700 悬浮颗粒物子相中半衰期/h 170 550 1 700 1 700 1 700 1 700 1 700 气溶胶子相中半衰期/h 17 55 170 170 170 170 170 注：Kow为正辛醇/水分配系数 
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表 2 大九湖环境参数
Table 2. Regional environmental parameters of Dajiuhu
环境参数 数据值 来源 环境参数 数据值 来源 气相面积/m2 1.11×107 本研究 气相高度/m 1×103 文献[30] 水相面积/m2 1.11×106 本研究 水深/m 0.96 文献[36] 土壤相面积/m2 9.99×107 本研究 土壤深度/m 0.1 文献[30] 沉积物相面积/m2 1.11×106 本研究 沉积物深度/m 0.1 文献[30] 气相中颗粒物体积分数 2×10-11 文献[30] 水相中悬浮颗粒物体积分数 5×10-6 文献[30] 水相中鱼的体积分数 1×10-6 文献[30] 土壤相水子相体积分数 0.3 文献[30] 土壤相气子相体积分数 0.2 文献[30] 土壤相颗粒物体积分数 0.5 文献[30] 沉积物相颗粒物体积分数 0.3 文献[30] 沉积物相水子相体积分数 0.7 文献[30] 大气相气子相密度/(kg·m-3) 1.185 文献[30] 大气相气溶胶密度/(kg·m-3) 2 000 文献[30] 水的密度/(kg·m-3) 1×103 文献[30] 水相中悬浮颗粒物密度/(kg·m-3) 1 030 文献[18] 水相中鱼的密度/(kg·m-3) 1×103 文献[30] 土壤相中颗粒物密度(kg·m-3) 2.4×103 文献[30] 沉积物中颗粒物密度/(kg·m-3) 2.4×103 文献[30] 土壤中有机碳质量分数/(g·g-1) 3×10-2 文献[37] 沉积物中有机碳质量分数/(g·g-1) 0.4 文献[34] 悬浮颗粒物有机碳质量分数/(g·g-1) 0.2 文献[30] 鱼的脂肪含量/(g·g-1) 0.05 文献[30] 气相侧气水质量迁移系数MTC/(m·h-1) 0.5 文献[30] 水相侧气水MTC/(m·h-1) 0.05 文献[30] 降雨速率/(m·h-1) 1.76×10-4 本研究 干沉降速率/(m·h-1) 10 文献[30] 土壤相中气子相MTC/(m·h-1) 0.02 文献[30] 土壤相中水子相MTC/(m·h-1) 1×10-5 文献[30] 土壤-气相边界层MTC/(m·h-1) 5 文献[30] 沉积物中水子相MTC/(m·h-1) 0.000 1 文献[30] 沉积物沉降速率/(m·h-1) 5×10-7 文献[30] 沉积物再悬浮速率/(m·h-1) 2×10-7 文献[30] 土壤相中水流失速率/(m·h-1) 5×10-5 文献[30] 土壤相中颗粒物流失速率/(m·h-1) 1×10-8 文献[30] 清洗速率/(m·h-1) 2×105 文献[30] 向气相排放速率/(kg·h-1) 0.001 本研究 污水排放速率/(m·h-1) 0.001 本研究 向土壤相排放速率/(m·h-1) 0.001 本研究 向沉积物相排放速率/(m·h-1) 0.001 本研究 气相中平流输入质量浓度/(ng·m-3) 20 文献[35]
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