Preliminary study on temporal trend lag of organic pollutant concentrations in environmental media and its influencing factors
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摘要: 选择131种有机物，通过构建EQC（EQuilibrium Criterion）标准环境的四级多介质模型，得出四种排放场景下，环境介质中有机物浓度的时间变化特征.在大多数情况下，环境介质内有机物浓度的时间变化出现滞后，lgKOW和持久性高的有机物浓度变化滞后最明显.相关分析表明，持久性为水相、大气相和土壤相中滞后时间的主要影响因素，lgKOW和持久性为沉积物相中的主要影响因素.通过回归分析，得到了滞后时间的预测公式.若沉积物相属于有机物的"汇"，则其中有机物浓度变化会产生明显的滞后.上述研究结果为了解环境中有机物的迁移转化规律提供了理论依据.Abstract: 131 organic chemicals were used, and a level IV EQuilibrium Criterion (EQC) multimedia model was built. The model was applied to simulate temporal trends of organic chemical concentrations in environmental media using four emission scenarios. Results showed that temporal trends of organic chemical concentrations lagged behind their emissions in most cases, and organic chemicals with higher lgKOW and persistence showed the most obvious lag effect. Correlation analysis showed that persistence was the principal factor influencing the lag time in water, air, and soil; and lgKOW and persistence were the principal factors in sediment. Prediction formulas for lag time were obtained by regression analysis. If the sediment was a sink of organic chemicals, the lag effect would be distinct.The study can be employed to illustrate the theoretical transfer and transformation of organic chemicals in an environmental system.
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Key words:
- organic pollutant /
- lag /
- temporal trend /
- environmental media /
- environmental model
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表 1 参数定义
Tab. 1 Parameter definitions
参数 定义 单位 $Z_{1}$、$Z_{2}$、$Z_{3}$和$Z_{4}$ 水相、大气相、沉积物相和土壤相的逸度容量 mol$\cdot $Pa$^{-1}\cdot $m$^{-3}$ $V_{1}$、$V_{2}$、$V_{3}$和$V_{4}$ 水相、大气相、沉积物相和土壤相的体积 m$^{3}$ $f_{1}$、$f_{2}$、$f_{3}$和$f_{4}$ 水相、大气相、沉积物相和土壤相中有机物的逸度 Pa $E_{1}$、$E_{2}$、$E_{3}$和$E_{4}$ 水相、大气相、沉积物相和土壤相中有机物的排放速率函数 mol$\cdot $a$^{-1}$ $D_{21}$ 大气相-水相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{31}$ 沉积物相-水相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{41}$ 土壤相-水相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{12}$ 水相-大气相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{13}$ 水相-沉积物相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{42}$ 土壤相-大气相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{24}$ 大气相-土壤相迁移$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{1{\rm R}}$、$D_{2{\rm R}}$、$D_{3{\rm R}}$和$D_{4{\rm R}}$ 水相、大气相、沉积物相和土壤相中有机物的反应$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ $D_{\rm 1out}$和$D_{\rm 2out}$ 水相和大气相中的平流$D$值 mol$\cdot $Pa$^{-1}\cdot $a$^{-1}$ 
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表 3 模型输入参数
Tab. 3 Model input parameters
参数 单位 分子量 g$\cdot $mol$^{-1}$ 蒸汽压 Pa 水溶解度 g$\cdot $m$^{-3}$ lg$K_{OW}$ / 熔点 ℃ 水相中半衰期 a 大气相中半衰期 a 沉积物相中半衰期 a 土壤相中半衰期 a 水相中有机物的排放速率函数 mol$\cdot $a$^{-1}$ 大气相中有机物的排放速率函数 mol$\cdot $a$^{-1}$ 沉积物相中有机物的排放速率函数 mol$\cdot $a$^{-1}$ 土壤相中有机物的排放速率函数 mol$\cdot $a$^{-1}$
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表 4 有机物的分类及典型有机物的参数
Tab. 4 Classification of organic chemicals and parameters of typical organic chemicals
分类 水溶解度 蒸汽压 lg$K_{OW}$ 持久性 典型有机物名称 CAS 蒸汽压/Pa 水溶解度/(g$\cdot $m$^{-3})$ lg$K_{OW}$ 半衰期/h 大气相 水相 土壤相 沉积物相 1 高 高 高 高 碘代苯$^{\ast }$ 591-50-4 130 340 3.28 550 5 500 17 000 55 000 2 高 高 高 低 苯乙烯 100-42-5 880 300 3.05 5 170 550 1 700 3 高 高 低 高 三氟乙酸 76-05-1 1.47$\times $10$^{4}$ 1$\times $10$^{6}$ 0.5 1 700 55 000 55 000 55 000 4 高 高 低 低 乙酸乙烯酯 108-05-4 1.41$\times $10$^{4}$ 2$\times $10$^{4}$ 0.73 55 55 170 550 5 高 低 高 高 异丙甲草胺$^{\ast }$ 51218-45-2 4.2$\times $10$^{-3}$ 430 3.13 550 5 500 5 500 17 000 6 高 低 高 低 2-甲-4-氯丙酸 93-65-2 3.1$\times $10$^{-4}$ 620 3.94 17 170 170 1 700 7 低 高 高 高 六氯乙烷$^{\ast }$ 67-72-1 50 50 3.93 55 000 5 500 17 000 55 000 8 低 高 高 低 正己烷 110-54-3 2.02$\times $10$^{4}$ 9.5 4.11 17 550 1 700 5 500 9 高 低 低 高 涕灭威$^{\ast }$ 116-06-3 4$\times $10$^{-3}$ 6$\times $10$^{3}$ 1.1 55 5 500 17 000 55 000 10 高 低 低 低 胺甲萘 63-25-2 2.67$\times $10$^{-5}$ 120 2.36 55 170 550 1 700 11 低 高 低 高 苯甲醇$^{\ast }$ 100-51-6 12 80 1.1 5 500 5 500 5 500 17 000 12 低 高 低 低 苯甲醇 100-51-6 12 80 1.1 55 55 55 170 13 低 低 高 高 六氯苯 118-74-1 2.3$\times $10$^{-3}$ 5$\times $10$^{-3}$ 5.5 7 350 55 000 55 000 55 000 14 低 低 高 低 邻苯二甲酸二异辛酯 117-81-7 1.33$\times $10$^{-5}$ 0.285 5.11 55 170 550 1 700 15 低 低 低 高 全氟辛酸铵 3825-26-1 9.52$\times $10$^{-3}$ 43.34 1.94 55 000 55 000 55 000 55 000 16 低 低 低 低 秋兰姆 137-26-8 1.3$\times $10$^{-3}$ 30 1.73 170 170 550 1 700 注: *表示半衰期经过调整
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表 5 每个分类中典型有机物峰值浓度的滞后时间
Tab. 5 Lag time of peak concentration for typical organic chemicals of each classification
分类 排放场景编号 峰值浓度滞后时间/a 分类 排放场景编号 峰值浓度滞后时间/a 水相 大气相 土壤相 沉积物相 水相 大气相 土壤相 沉积物相 1 1 0.1 0.1 0.7 0.8 9 1 0.2 0.2 0.4 0.2 2 0.1 0 0.6 0.8 2 0.4 0 0.3 0.4 3 0.7 0.6 0.6 1.3 3 0.4 0.3 0.3 0.5 4 0.1 0.3 0.6 0.8 4 0.3 0 0.3 0.4 2 1 0 0 0.1 0.3 10 1 0.1 0.1 0.2 0.2 2 0 0 0.1 0.3 2 0.1 0 0.2 0.2 3 0.1 0.1 0.1 0.4 3 0.2 0.2 0.2 0.3 4 0 0 0.1 0.3 4 0.1 0 0.2 0.2 3 1 0.2 0.2 0.3 0.2 11 1 0.1 0.1 0.2 0.2 2 0.2 0 0.2 0.3 2 0.1 0 0.1 0.2 3 0.3 0.2 0.2 0.4 3 0.2 0.1 0.1 0.2 4 0.2 0.1 0.2 0.3 4 0.1 0.1 0.1 0.2 4 1 0 0 0.1 0.1 12 1 0 0 0.1 0.1 2 0 0 0 0.1 2 0 0 0 0.1 3 0 0 0 0.1 3 0 0 0 0.1 4 0 0 0 0.1 4 0 0 0 0.1 5 1 0.2 0.2 0.9 0.7 13 1 0.1 0.1 1.5 2.5 2 0.5 0 0.8 1.0 2 0.1 0 2.3 1.5 3 0.9 0.8 0.8 1.4 3 2.5 2.3 2.3 5.1 4 0.3 0 0.8 0.8 4 0.1 0.1 2.3 1.5 6 1 0.1 0.1 0.1 0.4 14 1 0.1 0.1 0.2 0.4 2 0.1 0 0.1 0.4 2 0.1 0 0.2 0.4 3 0.1 0.1 0.1 0.4 3 0.2 0.2 0.2 0.5 4 0.1 0 0.1 0.4 4 0.1 0 0.2 0.4 7 1 0.1 0.1 0.8 1.2 15 1 0.2 0.2 0.7 0.3 2 0.1 0 0.8 1.2 2 0.6 0 0.6 0.7 3 0.8 0.8 0.8 1.9 3 0.7 0.6 0.6 0.8 4 0.1 0.3 0.8 1.2 4 0.4 0.1 0.6 0.5 8 1 0.1 0.1 0.1 0.7 16 1 0.1 0.1 0.2 0.1 2 0.1 0 0 0.7 2 0.1 0 0.1 0.2 3 0.1 0 0 0.7 3 0.2 0.1 0.1 0.2 4 0.1 0 0 0.7 4 0.1 0 0.1 0.2
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表 6 滞后时间与四种分类参数的Spearman相关系数
Tab. 6 Spearman correlation coefficients between lag time and four classification parameters
排放场景编号 环境介质 蒸汽压 水溶解度 lg$K_{OW}$ 水相中半衰期 滞后时间 1 水 -0.174 0.140 -0.049 0.754** 大气 -0.174 0.140 -0.049 0.754** 土壤 -0.183 -0.144 0.213 0.801** 沉积物 -0.004 -0.342 0.841** 0.501* 2 水 -0.205 0.081 -0.010 0.747** 大气 NA NA NA NA 土壤 -0.286 -0.123 0.359 0.738** 沉积物 -0.035 -0.300 0.709** 0.669** 3 水 -0.191 -0.165 0.291 0.833** 大气 -0.286 -0.123 0.359 0.738** 土壤 -0.286 -0.123 0.359 0.738** 沉积物 -0.027 -0.302 0.672** 0.693** 4 水 -0.207 0.085 -0.020 0.748** 大气 0.289 -0.108 0.062 0.721** 土壤 -0.286 -0.123 0.359 0.738** 沉积物 -0.016 -0.305 0.721** 0.658** *表示相关性达显著水平($P<$0.05), **表示相关性达极显著水平($P<$0.01), NA表示场景2中, 大气相中的滞后时间均为0, 不能计算出相关系数
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表 7 EQC模型中滞后时间的预测公式
Tab. 7 Prediction formulas for lag time in EQC model
场景编号 介质 预测公式 $R$ 1 水 0.048 28 (lg水相中半衰期) -0.005 181 (lg蒸汽压) -0.047 1 0.795 大气 0.049 87 (lg水相中半衰期) -0.005 680 (lg蒸汽压) -0.045 9 0.825 土壤 0.601 1 (lg土壤相中半衰期) -0.183 1 (lg水溶解度) -1.003 0.783 沉积物 0.240 7 (lg沉积物相中半衰期) +0.209 85 (lg $K_{OW}) $-1.012 2 0.953 2 水 0.074 41 (lg水相中半衰期) -0.029 71 (lg$K_{OW}) $-0.018 8 (lg蒸汽压) 0.771 大气 NA / 土壤 0.411 2 (lg土壤相中半衰期) -0.162 0 (lg水溶解度) -0.537 0.889 沉积物 0.277 (lg沉积物相中半衰期) +0.194 7 (lg$K_{OW}) $-1.076 3 0.952 3 水 0.595 9 (lg土壤相中半衰期) +0.266 (lg$K_{OW}) $-2.179 0.794 大气 0.456 5 (lg土壤相中半衰期) +0.232 7 (lg$K_{OW}) $-1.707 0.859 土壤 0.401 7 (lg土壤相中半衰期) -0.166 4 (lg水溶解度) -0.507 0.887 沉积物 0.853 (lg沉积物相中半衰期) +0.668 7 (lg$K_{OW}) $-4.104 0.841 4 水 0.060 71 (lg水相中半衰期) -0.015 36 (lg$K_{OW}) $-001 171 (lg蒸汽压) -0.019 3 0.804 大气 0.034 59 (lg大气相中半衰期) +0.007 49 (lg蒸汽压) -0.031 6 0.617 土壤 0.4017 (lg土壤相中半衰期) -0.1664 (lg水溶解度) -0.507 0.887 沉积物 0.261 8 (lg沉积物相中半衰期) +0.201 08 (lg$K_{OW}) $-1.052 3 0.953 注: NA表示场景2中, 大气相中的滞后时间均为0, 不能得出预测公式
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表 8 每个分类中典型有机物的(${{D}}_{\bf 13}$- ${ D}_{31}-{ D}_{{3}{{\rm R}}}$)值
Tab. 8 ($D_{13}-D_{31}-D_{3R})$ values for typical organic chemicals of each classification
mol·Pa-1·a-1 分类 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 $D_{13}-D_{31}-D_{3R}$ 1.2$\times $10$^{8}$ -4.5$\times $10$^{7}$ -2.5$\times $10$^{7}$ -7.9$\times $10$^{7}$ 2.4$\times $10$^{12}$ -8.8$\times $10$^{14}$ 1.7$\times $10$^{8}$ -1.8$\times $10$^{4}$ -4.0$\times $10$^{11}$ -1.0$\times $10$^{14}$ -1.0$\times $10$^{7}$ -1.0$\times $10$^{9}$ 1.0$\times $10$^{10}$ -6.5$\times $10$^{13}$ -7.9$\times $10$^{8}$ -2.0$\times $10$^{11}$
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