Migration of Petroleum Pollutants in Strong Heterogeneous Vadose Zones
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摘要: 为深入分析强非均质性污染场地中石油烃的运移规律,探究石油烃类污染物在场地中的吸附、迁移及其影响因素,选取潮白河上游为典型研究区,受冲洪积扇条件控制,区域内包气带非均质性强,地下水埋深较大.采集污染场地包气带介质样品,分别装填原状土(0~20 mm)、细颗粒(< 2 mm)和粗颗粒(>4 mm)3种介质迁移柱,通过土柱淋滤试验表征石油烃在典型介质中的迁移特性;通过静态吸附试验和微生物降解试验识别石油烃迁移过程的关键影响因素,揭示多要素作用条件下的石油烃迁移规律.结果表明:原状土、细颗粒和粗颗粒这3种介质迁移柱出水中石油烃浓度均呈先下降、后波动上升、最终趋于稳定的趋势.3种介质对石油烃的吸附过程均呈现快吸附和慢吸附两个阶段,快吸附阶段发生在试验0~15 h内,完成了吸附的70%~80%;慢吸附阶段持续时间较长,吸附总量缓慢增加.固液比、温度和pH等要素对3种介质石油烃吸附性能的影响相对较小.微生物降解是慢吸附阶段石油烃浓度呈波动上升的主要原因,且在整个石油烃垂向迁移过程中,吸附作用对石油烃去除的贡献率为80%,微生物降解的贡献率为20%.研究显示,相对于微生物作用而言,强非均匀介质在石油烃类污染场地的污染物吸附和迁移过程中起关键控制作用.Abstract: In order to analyze the migration and explore the adsorption, migration and influencing factors of petroleum hydrocarbons in strongly heterogeneous contaminated sites, the upper Chaobai River was selected as a typical research area. Under the control of an alluvial fan, the research area was characterized by strong heterogeneity and deep-groundwater depth. Samples were collected from the vadose zone and a migration column was filled with undisturbed fine and coarse particles. The transport characteristics of petroleum pollutants in typical media were characterized by column leaching experiments. Static adsorption and microbial degradation experiments were carried out to study the important influencing factors of petroleum hydrocarbon pollutants and to reveal the migration under the action of multiple factors in these three media. The migration of petroleum hydrocarbons in the three media decreased initially, fluctuated and then tended to stability. The adsorption process could be divided into a rapid adsorption stage (0-15 h, with 70%-80% adsorption) and a slow adsorption stage with a slow total adsorption. The solid-liquid ratio, temperature and pH had a relatively small effect on the adsorption of petroleum hydrocarbons. Microbial degradation was the main reason for the fluctuation in the slow adsorption stage. In the petroleum hydrocarbon migration process, the contribution from medium adsorption was 80% and microbial degradation was 20%. The results showed that strongly heterogeneous medium rather than microbiological deterioration played a key role in the adsorption and migration of petroleum hydrocarbon pollutants at the site.
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Key words:
- soil petroleum hydrocarbon /
- vadose zone /
- migration /
- soil interception /
- micro-biological degradation
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表 1 淋滤试验土柱及填充介质参数
Table 1. Parameter list of soil column and packing medium for leaching experiment
土柱名称 介质类型 粒度/mm 含量/% 备注 Ⅰ 细颗粒 < 2 100 原状土过分选筛,介质粒径小于2 mm < 2 35 过大孔筛,剔除植物根系和难以填充的大颗粒砾石 Ⅱ 原状土 2~20 45 20 10 Ⅲ 粗颗粒 4~20 33.3 经筛选,取4~20 mm介质与>20 mm介质按1:2比例混合后填充 >20 66.7 表 2 吸附要素试验条件
Table 2. Settings of adsorption experiment conditions
影响因素 溶液体积/mL 初始质量浓度/(mg/L) 振荡温度/℃ 吸附介质质量/g 振荡时间/h pH 固液比 40 12.712 15 0.2、0.4、1.0、2.0、4.0 24 7 温度 40 12.712 5、15、25、35、45 1.0 24 7 pH 40 12.712 15 1.0 24 3、5、7、9、11 表 3 微生物降解试验用柱及填充介质参数
Table 3. Parameter list of soil column and packing medium for microbial degradation experiment
土柱编号 柱长/cm 内径/cm 厚度 处理方法 迁移作用 柱A 25 6 8 mm有机玻璃 灭菌(加入HgCl2) 吸附 柱B 25 6 8 mm有机玻璃 不灭菌 吸附-微生物降解 表 4 热力学试验数据拟合参数
Table 4. Thermodynamic experimental data fitting parameters
介质 Langmuir等温吸附模型 Freundlich等温吸附模型 KL/(L/g) Cm/(mg/L) R2 Kf 1/n R2 细颗粒 0.026 02 1.427 44 0.979 99 0.038 36 0.883 68 0.973 87 原状土 0.041 01 0.767 64 0.992 29 0.034 14 0.813 01 0.986 78 粗颗粒 0.030 16 0.66 120 0.983 93 0.021 27 0.855 26 0.979 38 注:KL为Langmuir等温吸附常数,L/g;Kf为Freundlich等温吸附常数;C m为吸附平衡时溶液中的石油烃浓度,mg/L;1/n为Freundlich常数;R为相关系数. -
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