乌梁素海结冰过程中污染物迁移机理及其应用研究
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摘要
湖泊是最重要的淡水资源之一,在国民经济发展中起到极为重要的作用。作为我国八大淡水湖之一的乌梁素海湖泊,是全球范围内半荒漠地区极为少见的具有很高生态效益的大型多功能湖泊。但是由于近年来气候变化和人类活动的干扰,使得乌梁素海污染日益严重,引起了社会的广泛关注,并开展了大量的研究。但这些研究大都在湖泊非冰封期进行的,而乌梁素海地处高纬度地区,冰封时间长,其污染特征必将有别于其他湖泊。该研究以乌梁素海为研究对象,紧扣乌梁素海冰封期长的特点,在对湖泊结冰过程中气象、水文等要素观测的基础上,研究湖泊结冰过程中污染物的迁移机理、效应及其在牧区饮水安全中的应用,得出如下结论：
(1)研制了用于现场采集冰芯、水样和沉积物的成套仪器和室内模拟装置。在综合现有的采样方法的基础上,论述该套仪器的适应性和可行性：冰芯采集器采样方便,解决了进口采样器价格昂贵的“瓶颈”问题；水样和沉积物采集器配合冰芯采集器使用,可以采集湖泊冰-水界面等各部位的水样和无扰动的柱状沉积物。
(2)通过分析野外观测数据可知：气温对冰下水温的影响不明显,而冰温随着气温的升高也有较明显的升高,且其随着冰层深度的增加温度逐渐升高；运用朱波夫半经验模型表达式FDD=0.002T2.0.2251T可以较好地描述负累积温度和冰厚度间的关系；湖冰生长期冰密度变化不明显,在消融期,冰密度随深度的增加有增大的趋势；随着冰的生长,冰体的层理结构逐渐变化；湖面水深及冰厚有呈良好的负相关关系,其相关系数为0.53；乌梁素海冰封期冰下水体几乎处于静止状态。
(3)通过采集冰生长过程中不同冰厚度不同位置的冰样和水样,分析其污染物的含量,从结晶学理论和热力学理论角度探讨各结冰过程中污染物的迁移机理。
绘制了TDS分布轮廓线,定性和定量地阐述结冰过程中TDS在冰-水-沉积物体系间的迁移机理和过程。结果表明,在冰生长过程,约有80%的TDS由冰层迁移至水层；在冰层内部,TDS的迁移只发生在冰的生长初期,而后几乎不再迁移：湖冰中TDS的含量随着冰厚度的增加而降低,两者呈负指数关系；在冰下水体内部,在浓度差的作用下,TDS由冰-水界面向水体迁移直至达到平衡：在水和沉积物之间,约有60440950kg(约为冰水迁移量的16.78%)的TDS由水体迁移至沉积物；冰-水界面和水-沉积物界面TDS的迁移通量与冰生长率之间呈较好的线性正相关关系。
通过绘制pH值的轮廓线研究了结冰过程中pH值的变化。结果表明,由于碳酸盐体系对水体PH值得缓冲作用,导致在冰生长过程中pH值并没有明显的变化规律,即不能用湖冰的排TDS机理来解释pH值的变化。
通过分析不同采样时间的上、中、下层冰及冰-水界面水、中层水、水-沉积物界面水中各形态氮、磷、叶绿素a, COD和BOD5的时空变化曲线,探讨各污染物在冰生长过程中的迁移机理。结果表明：冰生长过程对各污染物有不同的排斥效应,冰下污染物的浓度随着冰厚的增加而升高。冰下水体中TN、NO3-、NO2-、NH4+的浓度分别是对应冰体中的2.06、1.77、1.26、2.35倍；冰-水界面水中各形态氮的含量高于中层水、水-沉积物界面水中的,而中层水和水-沉积物界面水中各形态氮的含量相差不大；上层冰体各形态氮的含量高于中、下层冰体的,两者的差值随着冰厚的增加而减小,表明各形态氮在冰体内部发生了迁移。冰下水体中TP、DTP、PO43-的浓度分别是对应冰体中的1.50、1.57、1.82倍。冰下水体中叶绿素a的浓度是对应冰体中的1.64倍；冰-水界面水中叶绿素a的含量明显高于中层水、水-沉积物界面水中的；冰体中叶绿素a与TN、TP的变化并没有明显规律,而水体中三者变化规律基本一致。
湖冰对有机物的排斥效应明显高于其对无机物的。冰下水体中COD是其对应冰体中的3.13倍：中层冰的COD均值略高于上、下层冰体的,水体的沉淀作用使得水体中的COD由上至下逐渐升高。冰下水体中BOD5是其对应冰体中的3.24倍；下层冰的BOD5均值略高于上、中层冰体的,水-沉积物界面水的BOD5高于中层和水-沉积物界面水的。冰下水体的PBOD5/PCOD高于冰融水的,表明冰下水体的可生化性较高；不同采样时间和不同采样位置上COD与BOD5均呈较好的正相关关系。
(4)运用分形理论对乌梁素海湖泊结冰前、后的富营养化状态进行了评价,以探讨结冰过程的环境效应。结果表明,乌梁素海湖泊各采样点结冰前水体、结冰后冰体和水体的富营养状态分别为富营养、富营养和重富营养；结冰过程使得湖泊水体的富营养状态加重,而部分低营养状态的水被冻结在冰体中。针对湖泊冰封期的污染特征提出了可行的底泥疏浚、冷冻浓缩等湖泊富营养修复对策。
由于结冰过程中平衡分凝系数的不确定性,采用加权马尔可夫链对结冰过程中冰下水体的TDS浓度进行预测。其预测精度较高,能够满足预测的要求,可为环保部门提前制定水环境保护措施提供数据参考。
(5)针对我国牧区存在的饮水安全隐患及牧区丰富的自然冷能、太阳能和风能的优势条件,提出将结冰过程中污染物的迁移机理应用到牧区饮水中的构想,设计了牧区饮用水的处理流程,并在考察室内模拟方法可行性的基础上,对流程中的冰厚、冷冻温度、受冷面积与水深比、种冰的加入及冷冻级数等工艺参数进行优化。这可为保障牧区饮用水安全提供思路和参考。
Lake is one of the most important freshwater resources, which plays a very important role in national economic development. Ulansuhai Lake is one of the eight great freshwater lakes in China, is also a multi-function lake which is extremely rare in the semi-desert area in the whole world. Ulansuhai Lake is polluted more and more seriously recently because of the climate change and interference of human activities, which has attracted widespread attention of government and scholars. A large number of studies on Ulansuhai Lake have been carried out, most of which focused on ice-free period. But Ulansuhai Lake is located in high-latitude area, in which the ice season is longer and the characteristics of pollution must be different from the ice-free period. Focusing on longer ice season, Ulansuhai Lake is selected for study object to dicuss the migration mechanism and effect of pollutants in freezing process and its application in pastoral area for drinking water safety. The results could be concluded as follows:
(1) A complete set of instruments for collecting ice samples, water samples, sediment samples, and simulating in laboratory is developed. Compared to the existing sampling method, the adaptability and feasibility of these instruments are described:the ice drill is easy to use, which solves the crucial high-price problem of imported instrument; water and sediment samplers well combined with ice drill can collect samples at every part consist of water nearby ice-water interface and water-sediment interface, water in sediment pores, and core sediments without disturbance.
(2) The field observation data shows:The effect of temperature on the under-ice water temperature is not significant, while ice temperature significantly increases as temperature rises and as ice depth deepened. The empirical formula of Zubov model, that is, FDD=0.002T2-0.2251T, can well describe the relationship between cumulative freezing-degree-day and corresponding ice thickness. The ice density changes not significantly in freezing process, it increases as ice depth deepened. The bedding structure of ice changes gradually as ice thickness grows. There was a good negative correlation between water depth and ice thickness in Ulansuhai Lake, and its correlation coefficient is0.53. The under-ice water is almost still during the icebound season.
(3) Ice samples and water samples at different depths were collected as ice thickness grows. The pollutant content of samples were analyzed to dicuss the migration mechanism in freezing process by means of crystallography and thermodynamic theory.
TDS profiles are drawn to show the distribution of TDS and to describe TDS migration qualitatively and qualitatively. The results showed that between ice and water, about80%, that is360158400kg, TDS migrated from ice to water during-the whole growth period. Within ice layer, TDS migration only occurred during initial ice period, then stopped almost. The ice TDS decreased with increasing ice thickness, following a negative exponential-like trend. Within under-ice water, TDS migrated from ice-water interface to the entire water column under motive power of concentration difference until the water TDS was uniform. Between water and sediment,60440950kg (16.78%of360158400kg) TDS migrated from water to sediment. The fitting curves for transfer flux of both ice-water and water-sediment to growth rate displayed good linear positive correlation relation.
pH profiles are also drawn to describe the change of pH value in freezing process. The results showed that it was not significantly that pH value as ice thickness grows because of buffer effect of carbonate system, which made the change of pH value different from TDS.
The space-time curve of N, P, Chlorophyll a, COD and BOD5were drawn to elaborate the migration mechanism and effect in freezing process based on analyzing the content of samples from upper ice, middle ice, lower ice, water at ice-water interface and water-sediment interface and middle water at different ice thickness. The results showed that exclusion effect of freezing process on N, P, Chlorophyll a, COD and BOD5was different, and the concentration of them in under-ice water increased as ice thickness grows. The concentration of TN, NO3-, NO2-, NH4+in under-ice water was respectively2.06,1.77,1.26,2.35times of that in ice. The concentration of TN, NO3-, NO2-, NH4+in water at ice-water interface was higer than that in middle water and at water-sediment interface, while the concentration of the latter two position was similar. The concentration of TN, NO3-, NO2-, NH4+in upper ice was higer than that in middle ice and lower ice. The difference between the two decreases with the increase of ice thickness, which revealed various forms of nitrogen migrated within the ice. The concentration of TP, DTP, PO43-and Chlorophyll a in under-ice water was respectively1.50,1.57,1.82and1.64times of that in ice. The concentration of Chlorophyll a in water at ice-water interface was higer than that in middle water and at water-sediment interface. There was no obvious rule among the concentration of Chlorophyll a, TN and TP in ice, but they were consistent in water.
The exclusion effect of freezing process on organics was more obvious than that on inorganics. COD in under-ice water was3.13times of that in ice. COD in middle ice was higer than that in upper ice and lower ice while COD in water increased from top to bottom due to the sedimentary action. BOD5in under-ice water was3.24times of that in ice. BOD5in lower ice was higer than that in middle ice and upper ice. BOD5in water at water-sediment interface was higer than that in middle water and at ice-water interface. The PBOD5/PCOD in under-ice water was higher than that in ice, which revealed the biodegradability of under-ice water was better than that of ice. There was positive correlation between COD and BOD5in every sample.
(4) The eutrophic state of Ulansuhai Lake before and after icing was assessed by mean of fractal theory to discuss the environmental effect of freeaing process. The results showed that the eutrophic state of water before icing, ice and under-ice water was respectively eutrophication, eutrophication and heavy eutrophication, that is, freeaing process made the eutrophic state of Ulansuhai Lake more heave because part of cleaner water was freezed in ice. The result can provide theoretical basis and data support for sediment dredging that is an effective nutritious repair countermeasure.
The concentration of TDS in under-ice water in freezing process was forecasted by mean of weighted markov chain, which was accurate and able to meet the forecast requirements.
(5) The idea that freeze purification process can be used easily and widely in that was rich in cold energy, wind energy and solar energy but existed drinking water safety hazard was proposed. Furthermore, the purification process was designed. The operating parameters in the purification process, that was ice thickness, freezing temperature, rate of area and depth of container, ice seed and freezing series, were optimizated based on that the feasibility of laboratory simulation was verified. The purification process can provide reference for drinking water safety in pastoral area.
(1)研制了用于现场采集冰芯、水样和沉积物的成套仪器和室内模拟装置。在综合现有的采样方法的基础上,论述该套仪器的适应性和可行性：冰芯采集器采样方便,解决了进口采样器价格昂贵的“瓶颈”问题；水样和沉积物采集器配合冰芯采集器使用,可以采集湖泊冰-水界面等各部位的水样和无扰动的柱状沉积物。
(2)通过分析野外观测数据可知：气温对冰下水温的影响不明显,而冰温随着气温的升高也有较明显的升高,且其随着冰层深度的增加温度逐渐升高；运用朱波夫半经验模型表达式FDD=0.002T2.0.2251T可以较好地描述负累积温度和冰厚度间的关系；湖冰生长期冰密度变化不明显,在消融期,冰密度随深度的增加有增大的趋势；随着冰的生长,冰体的层理结构逐渐变化；湖面水深及冰厚有呈良好的负相关关系,其相关系数为0.53；乌梁素海冰封期冰下水体几乎处于静止状态。
(3)通过采集冰生长过程中不同冰厚度不同位置的冰样和水样,分析其污染物的含量,从结晶学理论和热力学理论角度探讨各结冰过程中污染物的迁移机理。
绘制了TDS分布轮廓线,定性和定量地阐述结冰过程中TDS在冰-水-沉积物体系间的迁移机理和过程。结果表明,在冰生长过程,约有80%的TDS由冰层迁移至水层；在冰层内部,TDS的迁移只发生在冰的生长初期,而后几乎不再迁移：湖冰中TDS的含量随着冰厚度的增加而降低,两者呈负指数关系；在冰下水体内部,在浓度差的作用下,TDS由冰-水界面向水体迁移直至达到平衡：在水和沉积物之间,约有60440950kg(约为冰水迁移量的16.78%)的TDS由水体迁移至沉积物；冰-水界面和水-沉积物界面TDS的迁移通量与冰生长率之间呈较好的线性正相关关系。
通过绘制pH值的轮廓线研究了结冰过程中pH值的变化。结果表明,由于碳酸盐体系对水体PH值得缓冲作用,导致在冰生长过程中pH值并没有明显的变化规律,即不能用湖冰的排TDS机理来解释pH值的变化。
通过分析不同采样时间的上、中、下层冰及冰-水界面水、中层水、水-沉积物界面水中各形态氮、磷、叶绿素a, COD和BOD5的时空变化曲线,探讨各污染物在冰生长过程中的迁移机理。结果表明：冰生长过程对各污染物有不同的排斥效应,冰下污染物的浓度随着冰厚的增加而升高。冰下水体中TN、NO3-、NO2-、NH4+的浓度分别是对应冰体中的2.06、1.77、1.26、2.35倍；冰-水界面水中各形态氮的含量高于中层水、水-沉积物界面水中的,而中层水和水-沉积物界面水中各形态氮的含量相差不大；上层冰体各形态氮的含量高于中、下层冰体的,两者的差值随着冰厚的增加而减小,表明各形态氮在冰体内部发生了迁移。冰下水体中TP、DTP、PO43-的浓度分别是对应冰体中的1.50、1.57、1.82倍。冰下水体中叶绿素a的浓度是对应冰体中的1.64倍；冰-水界面水中叶绿素a的含量明显高于中层水、水-沉积物界面水中的；冰体中叶绿素a与TN、TP的变化并没有明显规律,而水体中三者变化规律基本一致。
湖冰对有机物的排斥效应明显高于其对无机物的。冰下水体中COD是其对应冰体中的3.13倍：中层冰的COD均值略高于上、下层冰体的,水体的沉淀作用使得水体中的COD由上至下逐渐升高。冰下水体中BOD5是其对应冰体中的3.24倍；下层冰的BOD5均值略高于上、中层冰体的,水-沉积物界面水的BOD5高于中层和水-沉积物界面水的。冰下水体的PBOD5/PCOD高于冰融水的,表明冰下水体的可生化性较高；不同采样时间和不同采样位置上COD与BOD5均呈较好的正相关关系。
(4)运用分形理论对乌梁素海湖泊结冰前、后的富营养化状态进行了评价,以探讨结冰过程的环境效应。结果表明,乌梁素海湖泊各采样点结冰前水体、结冰后冰体和水体的富营养状态分别为富营养、富营养和重富营养；结冰过程使得湖泊水体的富营养状态加重,而部分低营养状态的水被冻结在冰体中。针对湖泊冰封期的污染特征提出了可行的底泥疏浚、冷冻浓缩等湖泊富营养修复对策。
由于结冰过程中平衡分凝系数的不确定性,采用加权马尔可夫链对结冰过程中冰下水体的TDS浓度进行预测。其预测精度较高,能够满足预测的要求,可为环保部门提前制定水环境保护措施提供数据参考。
(5)针对我国牧区存在的饮水安全隐患及牧区丰富的自然冷能、太阳能和风能的优势条件,提出将结冰过程中污染物的迁移机理应用到牧区饮水中的构想,设计了牧区饮用水的处理流程,并在考察室内模拟方法可行性的基础上,对流程中的冰厚、冷冻温度、受冷面积与水深比、种冰的加入及冷冻级数等工艺参数进行优化。这可为保障牧区饮用水安全提供思路和参考。
Lake is one of the most important freshwater resources, which plays a very important role in national economic development. Ulansuhai Lake is one of the eight great freshwater lakes in China, is also a multi-function lake which is extremely rare in the semi-desert area in the whole world. Ulansuhai Lake is polluted more and more seriously recently because of the climate change and interference of human activities, which has attracted widespread attention of government and scholars. A large number of studies on Ulansuhai Lake have been carried out, most of which focused on ice-free period. But Ulansuhai Lake is located in high-latitude area, in which the ice season is longer and the characteristics of pollution must be different from the ice-free period. Focusing on longer ice season, Ulansuhai Lake is selected for study object to dicuss the migration mechanism and effect of pollutants in freezing process and its application in pastoral area for drinking water safety. The results could be concluded as follows:
(1) A complete set of instruments for collecting ice samples, water samples, sediment samples, and simulating in laboratory is developed. Compared to the existing sampling method, the adaptability and feasibility of these instruments are described:the ice drill is easy to use, which solves the crucial high-price problem of imported instrument; water and sediment samplers well combined with ice drill can collect samples at every part consist of water nearby ice-water interface and water-sediment interface, water in sediment pores, and core sediments without disturbance.
(2) The field observation data shows:The effect of temperature on the under-ice water temperature is not significant, while ice temperature significantly increases as temperature rises and as ice depth deepened. The empirical formula of Zubov model, that is, FDD=0.002T2-0.2251T, can well describe the relationship between cumulative freezing-degree-day and corresponding ice thickness. The ice density changes not significantly in freezing process, it increases as ice depth deepened. The bedding structure of ice changes gradually as ice thickness grows. There was a good negative correlation between water depth and ice thickness in Ulansuhai Lake, and its correlation coefficient is0.53. The under-ice water is almost still during the icebound season.
(3) Ice samples and water samples at different depths were collected as ice thickness grows. The pollutant content of samples were analyzed to dicuss the migration mechanism in freezing process by means of crystallography and thermodynamic theory.
TDS profiles are drawn to show the distribution of TDS and to describe TDS migration qualitatively and qualitatively. The results showed that between ice and water, about80%, that is360158400kg, TDS migrated from ice to water during-the whole growth period. Within ice layer, TDS migration only occurred during initial ice period, then stopped almost. The ice TDS decreased with increasing ice thickness, following a negative exponential-like trend. Within under-ice water, TDS migrated from ice-water interface to the entire water column under motive power of concentration difference until the water TDS was uniform. Between water and sediment,60440950kg (16.78%of360158400kg) TDS migrated from water to sediment. The fitting curves for transfer flux of both ice-water and water-sediment to growth rate displayed good linear positive correlation relation.
pH profiles are also drawn to describe the change of pH value in freezing process. The results showed that it was not significantly that pH value as ice thickness grows because of buffer effect of carbonate system, which made the change of pH value different from TDS.
The space-time curve of N, P, Chlorophyll a, COD and BOD5were drawn to elaborate the migration mechanism and effect in freezing process based on analyzing the content of samples from upper ice, middle ice, lower ice, water at ice-water interface and water-sediment interface and middle water at different ice thickness. The results showed that exclusion effect of freezing process on N, P, Chlorophyll a, COD and BOD5was different, and the concentration of them in under-ice water increased as ice thickness grows. The concentration of TN, NO3-, NO2-, NH4+in under-ice water was respectively2.06,1.77,1.26,2.35times of that in ice. The concentration of TN, NO3-, NO2-, NH4+in water at ice-water interface was higer than that in middle water and at water-sediment interface, while the concentration of the latter two position was similar. The concentration of TN, NO3-, NO2-, NH4+in upper ice was higer than that in middle ice and lower ice. The difference between the two decreases with the increase of ice thickness, which revealed various forms of nitrogen migrated within the ice. The concentration of TP, DTP, PO43-and Chlorophyll a in under-ice water was respectively1.50,1.57,1.82and1.64times of that in ice. The concentration of Chlorophyll a in water at ice-water interface was higer than that in middle water and at water-sediment interface. There was no obvious rule among the concentration of Chlorophyll a, TN and TP in ice, but they were consistent in water.
The exclusion effect of freezing process on organics was more obvious than that on inorganics. COD in under-ice water was3.13times of that in ice. COD in middle ice was higer than that in upper ice and lower ice while COD in water increased from top to bottom due to the sedimentary action. BOD5in under-ice water was3.24times of that in ice. BOD5in lower ice was higer than that in middle ice and upper ice. BOD5in water at water-sediment interface was higer than that in middle water and at ice-water interface. The PBOD5/PCOD in under-ice water was higher than that in ice, which revealed the biodegradability of under-ice water was better than that of ice. There was positive correlation between COD and BOD5in every sample.
(4) The eutrophic state of Ulansuhai Lake before and after icing was assessed by mean of fractal theory to discuss the environmental effect of freeaing process. The results showed that the eutrophic state of water before icing, ice and under-ice water was respectively eutrophication, eutrophication and heavy eutrophication, that is, freeaing process made the eutrophic state of Ulansuhai Lake more heave because part of cleaner water was freezed in ice. The result can provide theoretical basis and data support for sediment dredging that is an effective nutritious repair countermeasure.
The concentration of TDS in under-ice water in freezing process was forecasted by mean of weighted markov chain, which was accurate and able to meet the forecast requirements.
(5) The idea that freeze purification process can be used easily and widely in that was rich in cold energy, wind energy and solar energy but existed drinking water safety hazard was proposed. Furthermore, the purification process was designed. The operating parameters in the purification process, that was ice thickness, freezing temperature, rate of area and depth of container, ice seed and freezing series, were optimizated based on that the feasibility of laboratory simulation was verified. The purification process can provide reference for drinking water safety in pastoral area.
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