非饱和含水介质中石油污染物迁移—转化与淋洗技术研究
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摘要
伴随着石油的大规模勘探、开采,石油化工业的发展及其产品的广泛应用,石油对环境的污染已成为不容忽视的问题。石油进入到环境中后将经历挥发、淋溶、吸附和生物降解等一系列行为,而这些行为决定着石油污染物在环境中的归属。因此,深入研究石油污染物在环境中的迁移转化规律及其归属问题,对石油污染场地的评估、控制和修复具有重要的科学意义和应用价值。
本研究以取自淄博市的壤土和砂土作为含水介质,选择柴油和汽油为供试油品。通过研究含水介质中石油挥发、淋溶和残留行为；研究不同水溶液条件引起的油水界面张力变化及其对化学淋洗效果的影响,取得了一些新的认识和结论：
(1)含水介质中石油挥发速率与含油率、风速、容器直径、挥发土样厚度和介质颗粒粒径有关,汽油和柴油的挥发过程可分别用Elovich方程和抛物线模型描述。风加快含水介质中汽油和柴油挥发速率,使柴油中nC9-nC15组分挥发加快,但nC16的挥发受影响小。柴油挥发速率系数分别与容器直径和挥发土样厚度呈线性正相关,而容器直径对汽油挥发影响不明显,增加挥发土样厚度使汽油挥发速率降低。含水介质的颗粒越细,柴油挥发越快,而含水介质则抑制了汽油的挥发,且颗粒越细的含水介质中汽油挥发越慢。粗砂中水分可加快柴油挥发,细砂和亚粘土中水分却使柴油挥发速率减慢。在挥发过程中,柴油中低碳组分逐渐消失,高碳组分的相对含量增大。
(2)颗粒大小和堆积密度影响含水介质中石油挥发和淋溶过程。当含水介质中石油挥发达到平衡后,亚粘土、细砂和粗砂中石油挥发量依次减少。相同介质中,石油在堆积密度小粗砂中挥发更快,而在堆积密度小的亚粘土中挥发较慢,堆积密度对细砂中石油挥发影响不大。在水淋滤过程中,粗砂中石油释放最快。在随后的反复多次清洗下,亚粘土中石油极限残留量是粗砂的20多倍。
(3)石油在含水介质中含量和组分分布因含水介质性质和深度而有所不同。粗砂柱的最上层和底层的石油含量较高,中部石油含量相对较低,亚粘土柱的最上层石油含量最低,在其下层的石油含量最高。不同深度粗砂中柴油的nC20、nC21、nC18和nC17相对含量较高,而亚粘土中柴油的nC16和nC15相对含量最高。
(4)石油最大残留饱和度、稳定残留饱和度和极限残留量与含水介质的颗粒粒径、有机质含量和比表面积等有关。颗粒均匀含水介质中石油最大残留饱和度、稳定残留饱和度和极限残留量均随平均粒径的增大而减小,粒径范围广含水介质中石油最大残留饱和度同样与介质平均粒径有关,但石油稳定残留饱和度与有机质含量和比表面积关系密切。堆积密度影响颗粒均匀含水介质中石油最大残留饱和度的大小,而对石油稳定残留饱和度的影响较小。
(5)初始水饱和度影响含水介质中石油残留饱和度的大小。初始水饱和度增加使含水介质中石油饱和度降低,但对颗粒均匀含水介质中石油稳定残留饱和度影响较小。当含水介质初始水饱和度大于临界水饱和度时,油水总饱和度为一定值,而当初始水饱和度小于临界水饱和度时,油水总饱和度将随初始水饱和度增加而增加。
(6)水溶液性质变化、无机盐和有机溶剂的加入对油水界面张力产生不同程度的影响,而无机盐、有机溶剂和阴离子表面活性剂的加入能提高单一表面活性剂的去油效果。化学淋洗油污砂土的静态和土柱试验表明,氯化钙、SDS和有机溶剂分别与Triton X-100混用,其去油率高于单一表面活性剂Triton X-100的去油率,且增效作用依次增大。从3因素对Triton X-100的综合作用静态试验结果分析,各因素的主次顺序为：丙酮>SDS＞CaCl2。在4因素淋洗油污砂柱正交试验中,得到各因素的主次顺序为：CaCl2＞温度>流量>pH。
With the large-scale oil exploration, mining, development of petroleum chemical industry and widely use of its products, oil pollution to environment cannot be ignored. After entering into environment, oil contaminants undergo a series of acts, such as volatilization, leaching, adsorption and biological degradation, which determine the ultimate fate of oil contaminants in environment. Therefore, it has important scientific significance and application value for assessment, control and remediation of oil-contaminated fields to research the migration, transformation and the final fate of oil contaminants deeply.
In this paper, loam and sand were taken as representative aquifer media, and diesel oil and gasoline were chosen as the pollutants. The oil volatilization, leaching and residual behaviors were studied. Different solution conditions caused the change of oil-water interfacial tension, which affected the chemical leaching efficiency at the same time. On the basis of these investigation and experimental tests, some conclusions can be summarized as follows:
(1) The volatilization rates of oil on aquifer media are relevant to oil content, wind speed, vessel diameter, volatilization thickness and particle size. Elovich equation and parabolic model can express the volatilization process of gasoline and diesel oil in aquifer media respectively. The wind can accelerate the volatilization rate of oils. The wind can speed up the volatilization of nC9～nC15of diesel oil significantly, but has little effect on the volatilization of nC16. Linear equations can describe the increment of diesel oil volatilization coefficients with the increasing of volatilization thickness and vessel diameter. But vessel diameter has no significant effect on gasoline volatilization, and the increasing volatilization thickness makes gasoline volatilization rate slow down. The finer is the aquifer media particle size, the faster diesel oil volatizes. But aquifer media block the gasoline volatilization, and gasoline in fine grained aquifer media volatilizes slower. The water in coarse sand can speed up the diesel oil volatilization, while which in fine sand and loam reduce the diesel oil volatilization rate. In the oil volatilization process, the low-carbon components disappear gradually, the relative contents of high-carbon components increase.
(2) The particle size and bulk density of aquifer media affect oil volatilization and washing process. When the oil volatilization in aquifer media reaches equilibrium, the oil volatilization losses in coarse sand, fine sand and loam increase in turn. In the same aquifer media, oils in coarse sand and loam under lower bulk density volatilize faster and slower respectively, and the bulk density has little effect on the oil volatilization in fine sand. The oil releases fastest in coarse sand with water leaching. The minimum oil content of loam is20times than that of coarse sand under the water washing repeatedly.
(3) The oil content and oil components in vadose zone soil distribute differently because of the different aquifer media characteristic and soil depth. The oil content of top and bottom layers is higher for coarse sand column, and the oil content of central layer is relatively lower. For loam column, the oil content of top layer is lowest, and the oil content of the layer under top layer is highest. The relative contents of nC2o, nC21, nC18and nC17are relatively higher in different depth of coarse sand column, but the relative contents of nC16and nC15are highest for loam column.
(4) The particle size, organic matter content and specific surface area of aquifer media affect the maximum residual oil saturation, stable residual oil saturation and minimum oil content. The maximum residual oil saturation, stable residual oil saturation and minimum oil content of homogeneous aquifer media decrease with the increase of mean grain size. Mean grain size of heterogeneous aquifer media is the main factor affectting maximum residual oil saturation, while the stable residual oil saturation is related to organic matter content and specific surface area. Bulk density of homogeneous aquifer media affects the maximum residual oil saturation, but its effect on stable residual oil saturation is little.
(5) The residual oil saturation is related to the initial water saturation of aquifer media. The increasing of initial water saturation can result in residual oil saturation in aquifer media reducing, but which has little effect on the residual oil saturation of homogeneous aquifer media. When the initial water saturation is greater than the critical water saturation, the total saturation of oil and water is a constant value, but when the initial water saturation is less than the critical water saturation, the total saturation increases with increasing of initial water saturation.
(5) The change of solution properties, the adding of inorganic salt and organic solvent affect the oil-water interfical tension. The intruduction of inorganic salt, organic solvent and anionic surfactant can improve the oil removal efficiency of sole surfactant. The chemical leaching experiments show that the oil removal rates of mixed solvent are higher than the single Triton X-100. The improvement effects of CaCl2, SDS and organic increase in turn. The composite effect of the three factors on the oil removal rate of Triton X-100is Acetone>SDS> CaCl2in orthogonal test. While the effect of the four factors on the oil removal rate of water is CaCl2＞temperature＞flow velocity＞pH.
本研究以取自淄博市的壤土和砂土作为含水介质,选择柴油和汽油为供试油品。通过研究含水介质中石油挥发、淋溶和残留行为；研究不同水溶液条件引起的油水界面张力变化及其对化学淋洗效果的影响,取得了一些新的认识和结论：
(1)含水介质中石油挥发速率与含油率、风速、容器直径、挥发土样厚度和介质颗粒粒径有关,汽油和柴油的挥发过程可分别用Elovich方程和抛物线模型描述。风加快含水介质中汽油和柴油挥发速率,使柴油中nC9-nC15组分挥发加快,但nC16的挥发受影响小。柴油挥发速率系数分别与容器直径和挥发土样厚度呈线性正相关,而容器直径对汽油挥发影响不明显,增加挥发土样厚度使汽油挥发速率降低。含水介质的颗粒越细,柴油挥发越快,而含水介质则抑制了汽油的挥发,且颗粒越细的含水介质中汽油挥发越慢。粗砂中水分可加快柴油挥发,细砂和亚粘土中水分却使柴油挥发速率减慢。在挥发过程中,柴油中低碳组分逐渐消失,高碳组分的相对含量增大。
(2)颗粒大小和堆积密度影响含水介质中石油挥发和淋溶过程。当含水介质中石油挥发达到平衡后,亚粘土、细砂和粗砂中石油挥发量依次减少。相同介质中,石油在堆积密度小粗砂中挥发更快,而在堆积密度小的亚粘土中挥发较慢,堆积密度对细砂中石油挥发影响不大。在水淋滤过程中,粗砂中石油释放最快。在随后的反复多次清洗下,亚粘土中石油极限残留量是粗砂的20多倍。
(3)石油在含水介质中含量和组分分布因含水介质性质和深度而有所不同。粗砂柱的最上层和底层的石油含量较高,中部石油含量相对较低,亚粘土柱的最上层石油含量最低,在其下层的石油含量最高。不同深度粗砂中柴油的nC20、nC21、nC18和nC17相对含量较高,而亚粘土中柴油的nC16和nC15相对含量最高。
(4)石油最大残留饱和度、稳定残留饱和度和极限残留量与含水介质的颗粒粒径、有机质含量和比表面积等有关。颗粒均匀含水介质中石油最大残留饱和度、稳定残留饱和度和极限残留量均随平均粒径的增大而减小,粒径范围广含水介质中石油最大残留饱和度同样与介质平均粒径有关,但石油稳定残留饱和度与有机质含量和比表面积关系密切。堆积密度影响颗粒均匀含水介质中石油最大残留饱和度的大小,而对石油稳定残留饱和度的影响较小。
(5)初始水饱和度影响含水介质中石油残留饱和度的大小。初始水饱和度增加使含水介质中石油饱和度降低,但对颗粒均匀含水介质中石油稳定残留饱和度影响较小。当含水介质初始水饱和度大于临界水饱和度时,油水总饱和度为一定值,而当初始水饱和度小于临界水饱和度时,油水总饱和度将随初始水饱和度增加而增加。
(6)水溶液性质变化、无机盐和有机溶剂的加入对油水界面张力产生不同程度的影响,而无机盐、有机溶剂和阴离子表面活性剂的加入能提高单一表面活性剂的去油效果。化学淋洗油污砂土的静态和土柱试验表明,氯化钙、SDS和有机溶剂分别与Triton X-100混用,其去油率高于单一表面活性剂Triton X-100的去油率,且增效作用依次增大。从3因素对Triton X-100的综合作用静态试验结果分析,各因素的主次顺序为：丙酮>SDS＞CaCl2。在4因素淋洗油污砂柱正交试验中,得到各因素的主次顺序为：CaCl2＞温度>流量>pH。
With the large-scale oil exploration, mining, development of petroleum chemical industry and widely use of its products, oil pollution to environment cannot be ignored. After entering into environment, oil contaminants undergo a series of acts, such as volatilization, leaching, adsorption and biological degradation, which determine the ultimate fate of oil contaminants in environment. Therefore, it has important scientific significance and application value for assessment, control and remediation of oil-contaminated fields to research the migration, transformation and the final fate of oil contaminants deeply.
In this paper, loam and sand were taken as representative aquifer media, and diesel oil and gasoline were chosen as the pollutants. The oil volatilization, leaching and residual behaviors were studied. Different solution conditions caused the change of oil-water interfacial tension, which affected the chemical leaching efficiency at the same time. On the basis of these investigation and experimental tests, some conclusions can be summarized as follows:
(1) The volatilization rates of oil on aquifer media are relevant to oil content, wind speed, vessel diameter, volatilization thickness and particle size. Elovich equation and parabolic model can express the volatilization process of gasoline and diesel oil in aquifer media respectively. The wind can accelerate the volatilization rate of oils. The wind can speed up the volatilization of nC9～nC15of diesel oil significantly, but has little effect on the volatilization of nC16. Linear equations can describe the increment of diesel oil volatilization coefficients with the increasing of volatilization thickness and vessel diameter. But vessel diameter has no significant effect on gasoline volatilization, and the increasing volatilization thickness makes gasoline volatilization rate slow down. The finer is the aquifer media particle size, the faster diesel oil volatizes. But aquifer media block the gasoline volatilization, and gasoline in fine grained aquifer media volatilizes slower. The water in coarse sand can speed up the diesel oil volatilization, while which in fine sand and loam reduce the diesel oil volatilization rate. In the oil volatilization process, the low-carbon components disappear gradually, the relative contents of high-carbon components increase.
(2) The particle size and bulk density of aquifer media affect oil volatilization and washing process. When the oil volatilization in aquifer media reaches equilibrium, the oil volatilization losses in coarse sand, fine sand and loam increase in turn. In the same aquifer media, oils in coarse sand and loam under lower bulk density volatilize faster and slower respectively, and the bulk density has little effect on the oil volatilization in fine sand. The oil releases fastest in coarse sand with water leaching. The minimum oil content of loam is20times than that of coarse sand under the water washing repeatedly.
(3) The oil content and oil components in vadose zone soil distribute differently because of the different aquifer media characteristic and soil depth. The oil content of top and bottom layers is higher for coarse sand column, and the oil content of central layer is relatively lower. For loam column, the oil content of top layer is lowest, and the oil content of the layer under top layer is highest. The relative contents of nC2o, nC21, nC18and nC17are relatively higher in different depth of coarse sand column, but the relative contents of nC16and nC15are highest for loam column.
(4) The particle size, organic matter content and specific surface area of aquifer media affect the maximum residual oil saturation, stable residual oil saturation and minimum oil content. The maximum residual oil saturation, stable residual oil saturation and minimum oil content of homogeneous aquifer media decrease with the increase of mean grain size. Mean grain size of heterogeneous aquifer media is the main factor affectting maximum residual oil saturation, while the stable residual oil saturation is related to organic matter content and specific surface area. Bulk density of homogeneous aquifer media affects the maximum residual oil saturation, but its effect on stable residual oil saturation is little.
(5) The residual oil saturation is related to the initial water saturation of aquifer media. The increasing of initial water saturation can result in residual oil saturation in aquifer media reducing, but which has little effect on the residual oil saturation of homogeneous aquifer media. When the initial water saturation is greater than the critical water saturation, the total saturation of oil and water is a constant value, but when the initial water saturation is less than the critical water saturation, the total saturation increases with increasing of initial water saturation.
(5) The change of solution properties, the adding of inorganic salt and organic solvent affect the oil-water interfical tension. The intruduction of inorganic salt, organic solvent and anionic surfactant can improve the oil removal efficiency of sole surfactant. The chemical leaching experiments show that the oil removal rates of mixed solvent are higher than the single Triton X-100. The improvement effects of CaCl2, SDS and organic increase in turn. The composite effect of the three factors on the oil removal rate of Triton X-100is Acetone>SDS> CaCl2in orthogonal test. While the effect of the four factors on the oil removal rate of water is CaCl2＞temperature＞flow velocity＞pH.
引文
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