煤矸石淋溶液对地下水系统污染规律的研究
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摘要
本文基于前人研究成果基础之上,运用地下水动力学、多孔介质流体力学、环境化学以及水文地质学等多学科相关理论,利用理论、实验和数值模拟相结合的方法,对煤矸石淋溶液对地下水系统污染机理和规律进行了较深入地研究:
(1)通过室内煤矸石静、动态淋溶实验研究,科学、全面、系统、深入地揭示了新邱露天矿不同风化程度煤矸石在水岩相互作用下溶解释放出的主要污染组分为总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠(Na~+)、总溶解性固体(TDS)等,这一结果与Szcepanska对波兰380余座煤矸石山进行的调查研究发现煤矸石的主要污染是盐度、含硫量和潜在的酸性等基本是一致的;揭示了煤矸石在长期的地球物理、化学风化、自然降水淋溶等作用下随着大量黄铁矿的氧化、分解、溶解反应以及碳酸盐岩、硅铝酸盐岩矿物的溶解反应使煤矸石风化,风化程度越高的煤矸石在水岩相互作用下溶解释放的总硬度、硫酸盐、钠、总溶解性固体等无机污染物量越多的内在机制;揭示了影响煤矸石污染组分溶解释放的主要因素为固液比、浸泡时间、酸度、搅动、矸石粒度大小以及水的动态流动等;提出了煤矸石在水岩相互作用下主要污染组分溶解释放的多相反应动力学机理即:整个溶解过程分为两个阶段:①是易溶组分脱离界面过程;②是脱离界面后以低速向外扩散过程。且溶解扩散服从菲克(Fick)扩散定律;建立了煤矸石在动态淋溶作用下主要污染组分溶解释放规律的数学模型:Cv=C_0V~n,从而可定量预测煤矸石中主要污染组分在大气降水作用下对地下水系统污染的强度;
(2)通过室内土柱动态模拟试验,研究揭示了煤矸石淋溶液主要污染组分总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2+))、钠(Na~+)在地下水系统中的多组分运移机理和污染规律:总硬度(Ca~(2+)+Mg~(2+))的运移速度很快,硫酸盐(SO_4~(2-))次之,而钠离子(Na~+)的运移速度最慢;对流、水动力弥散和吸附作用是造成总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))和钠离子(Na~+)运移的主要原因,对污染组分的运移起主要作用;土壤介质对总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))和钠离子(Na~+)都发生了吸附作用,且吸附强弱不同,对钠离子(Na~+)的吸附最强,硫酸盐(SO_4~(2-))次之,而对总硬度(Ca~(2+)+Mg~(2+))的吸附较弱,且土壤介质对三者的吸附都符合线性等温平衡吸附规律。并测定了土壤的渗透系数、水动力弥散系数以及总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠(Na~+)在饱水砂性土壤中的吸附分配系数(cm~3/g)和迟滞因子分别为1.59×10~(-2)cm~3/g、6.5×10~(-2)cm~3/g、4.22×10~(-1)cm~3/g和1.08、1.34、3.21,为模型的验证和数值模拟提供了可靠的实测参数;
(3)系统地分析了影响污染组分运移的主要因素,建立了综合考虑对流、水动力弥散、吸附解吸及存在源汇项条件下的定量描述土壤-地下水系统中主要污染组分运移三维动力学耦合数学模型,利用有限差分方法对数学模型进行了数值离散,给出了数值解法;
(4)利用数值模拟方法,对煤矸石淋溶液中主要污染组分总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠离子(Na~+)在研究区域地下水系统中的浓度时空分布规律进行了三维数值模拟研究,结果表明:污染面积随时间推移不断向两轴方向扩大,且纵向显著,在地下水流的下方向,污染范围较大,地下水流的上方向,污染范围较小,地下水流的两侧方向,污染范围基本呈对称分布;污染组分浓度值向两轴方向逐次递减,淋溶液对地下水体污染程度与距污染源的距离有关,距离污染源越远,溶质的浓度越低;在垂向方向,污染组分随水流运移的同时逐渐向下方渗漏,污染面积不断扩大,并逐次递减,在污染源下部的0-20m深度范围内含量最高;而同一位置污染组分的浓度值随时间的延续呈逐渐增大的趋势,最后达到平衡;总硬度(Ca~(2+)+Mg~(2+))在地下水中运移的速度大于硫酸根的运移速度,更大于钠离子(Na~+)的运移速度;模拟相同时间后总硬度(Ca~(2+)+Mg~(2+))的运移范围较大,硫酸根(SO_4~(2-))的运移范围次之,而钠离子(Na~+)的运移范围最小,总硬度(Ca~(2+)+Mg~(2+))最先达到平衡,硫酸根(SO_4~(2-))次之,而钠离子(Na~+)的运移非常缓慢,所以总硬度(Ca~(2+)+Mg~(2+))、硫酸根(SO_4~(2-))污染的范围比钠离子(Na~+)污染的范围广,对地下水质破坏的程度比较严重;
(5)通过对新邱原南露天矿煤矸石山周围地区的地下水水质进行的调查、监测表明:该区地下水受到了严重污染,且污染源主要来自煤矸石山。煤矸石山是长期的污染源,是造成周围地区地下水无机盐类污染的主要原因。这一结论与波兰学者对380余座煤矸石山进行研究发现的煤矸石山是地下水污染的长期污染源以及煤矸石的主要污染是盐度、含硫量和潜在的酸性等基本是一致的;
(6)将数值模拟值与研究区域地下水多年的监测数据进行对比,进一步验证了所建数学模型的可靠性。该数学模型和数值模拟方法对其它地区煤矸石淋溶液对地下水系统污染问题普遍适用。
最后对煤矸石山淋溶液对地下水污染问题提出了治理措施。
本文的研究成果对于揭示煤矸石对地下水系统污染的环境动力学行为具有重要的科学理论意义,对地下水环境污染的预测、预报和管理具有重要的理论意义和实际意义,为更科学、更有效地预防、控制和治理矿区煤矸石固体废物排放带来的地下水系统污染问题提供了科学理论依据。
Based on the previous research results,the multi-disciplinary relevant theories of the groundwater dynamics,porous medium fluid dynamics, environmental chemistry and hydrogeology,and the combination of the theories, experiments and numerical simulation,this paper conducted a series of further investigations on pollution mechanism and laws of coal gangue leaching solution to groundwater system:
(1)The bench scale.soaking- leaching and dynamic leaching experiment indicates:the main pollution components released by the coal gangue of different rate of decay under water-rock interaction in Xinqiu open-cut mine are total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-)),sodium(Na~+)and total dissolved solid(TDS),the results of which are basically in accordance with the investigation of the 380 plus coal gangue hills in Poland conducted by Szcepanska;The coal gangue is eroded under geophysical function,chemical erosion and natural precipitation in the company of the oxidation, decomposition and dissolution reactions of the pyrite and the dissolution of the carbonate and aluminosilicate minerals.The higher the rate of decay is,the more pollution components the coal gangue releases;The main factors influencing the dissolution-release are the solid-liquid ratio,soak time,acidity, agitation,grain size and water dynamic flow.Moreover,heterogeneous reaction kinetics mechanism of the dissolution-release of the main pollution components was revealed,which abides by the Fick' s law;And builds the index fading equation of the dissolution-release regularity of the main pollution components and precipitation:C_v=C_0V~n,which can quantitatively predicts the pollution intensity of the main pollution components to groundwater system under atmospheric precipitation.
(2)The laboratory column dynamic simulating experiment reveals the multicomponent transport mechanism and pollution laws of the main pollution components of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+)in soil-groundwater system.That is,the transport velocity of the total hardness (Ca~(2+)+Mg~(2+))is the biggest followed by sulfate(SO_4~(2-)),and sodium(Na~+)the lowest.Namely,advection,mechanical dispersion and adsorption are the principal reasons of the transport of the total hardness(Ca~(2+)+Mg~(2+)), sulfate(SO_4~(2-))and sodium(Na~+)and play an vital role in the transport. Adsorption of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+) occurs in the soil medium,while the adsorption intensity is different.The adsorption of sodium(Na~+)is the strongest followed by sulfate(SO_4~(2-)),and total hardness(Ca~(2+)+Mg~(2+))the weakest.In general,their adsorption conforms to the linear equilibrium sorption isotherm.The soil conductivity,fluid dynamic dispersivity,adsorption distribution coefficient and retardation factor of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+)are also measured.The adsorption distribution coefficient and retardation factor for the three are 1.59×10-2 cm~3/g、6.5×10-2cm~3/g、4.22×10-1 cm~3/gand1.08,1.34,3.21,these offer measured parameters for model verification and numerical simulation.
(3)Systematically analyze the essential factors influencing the pollution component transport and build three-dimensional dynamic coupled numerical model to describe the transport of the main pollution components in soil-groundwater system under the consideration of advection,hydrodynamic dispersion,adsorption-desorption and source and sink.The model underwent numerical discretization using finite-difference and the numerical solution was given.
(4)Numerical simulation.was conducted to the concentration temporal and spatial distribution of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium (Na~+)in the groundwater system,the results of which indicate:The pollution area enlarges continuously with the passage of time and the longitudinal direction is more remarkable.The pollution scale is bigger in the groundwater downstream,smaller in the upstream,and distributes symmetrically on both sides;The pollutant concentration decreases gradually on either axis and the pollution degree of the leaching solution to the groundwater system is related to the distance of the pollution sources,the farther away from sources of pollution, the concentration of solute lower;In the vertical direction,with the current migration of contaminants at the same time gradually to the bottom of leaks, pollution area continued to expand,and successive decline.In the lower part of the pollution sources within 0-20m depth of the highest.The pollutant concentration in one location increases gradually with the passage of time and finally reaches equilibrium;The transport velocity of total hardness(Ca~(2+)+Mg~(2+)) is bigger than that of sulfate and much bigger than that of sodium;In the same simulation time period,the transport scale of total hardness(Ca~(2+)+Mg~(2+))is the largest and then sulfate(SO_4~(2-))and sodium(Na~+)sequentially.The total hardness(Ca~(2+)+Mg~(2+))comes to equilibrium first followed by sulfate(SO_4~(2-)) and sodium(Na~+)the slowest,so the pollution scale of hardness(Ca~(2+)+Mg~(2+)) and sulfate(SO_4~(2-))is larger than that of sodium(Na~+)and eventually causes more severe pollution to the groundwater.
(5)The investigation and monitoring to the water quality of groundwater in the surrounding areas of the coal gangue hills in formal Xinqiu open-cut mine demonstrate that the investigation areas have been polluted heavily by main pollution components of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-)),sodium(Na ~+)and total dissolved solid(TDS).The pollution sources is the coal gangue hill. The coal gangue hill is a long-term pollution source and is the main reason of groundwater inorganic salts pollution in the surrounding areas,which is also in accordance with the study conducted in Poland.
(6)The simulation results were compared with the many-year monitoring datas of the groundwater in the study region,which demonstrates that the mathematical model built is reliable.The model and numerical simulation method are also applicable to the pollution of inorganic salts to the groundwater in other regions.
In the end,the countermeasures were given to the groundwater pollution issues by coal gangue.
This study is of great scientific significance to reveal the environmental dynamics of the groundwater pollution by coal gangue.It is also of great theoretical and practical significance to predict,forecast and manage the groundwater pollution and lays theoretical foundations for preventing, controlling and treating the groundwater pollution issues caused by coal gangue in coal mine sites scientifically and efficiently.
(1)通过室内煤矸石静、动态淋溶实验研究,科学、全面、系统、深入地揭示了新邱露天矿不同风化程度煤矸石在水岩相互作用下溶解释放出的主要污染组分为总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠(Na~+)、总溶解性固体(TDS)等,这一结果与Szcepanska对波兰380余座煤矸石山进行的调查研究发现煤矸石的主要污染是盐度、含硫量和潜在的酸性等基本是一致的;揭示了煤矸石在长期的地球物理、化学风化、自然降水淋溶等作用下随着大量黄铁矿的氧化、分解、溶解反应以及碳酸盐岩、硅铝酸盐岩矿物的溶解反应使煤矸石风化,风化程度越高的煤矸石在水岩相互作用下溶解释放的总硬度、硫酸盐、钠、总溶解性固体等无机污染物量越多的内在机制;揭示了影响煤矸石污染组分溶解释放的主要因素为固液比、浸泡时间、酸度、搅动、矸石粒度大小以及水的动态流动等;提出了煤矸石在水岩相互作用下主要污染组分溶解释放的多相反应动力学机理即:整个溶解过程分为两个阶段:①是易溶组分脱离界面过程;②是脱离界面后以低速向外扩散过程。且溶解扩散服从菲克(Fick)扩散定律;建立了煤矸石在动态淋溶作用下主要污染组分溶解释放规律的数学模型:Cv=C_0V~n,从而可定量预测煤矸石中主要污染组分在大气降水作用下对地下水系统污染的强度;
(2)通过室内土柱动态模拟试验,研究揭示了煤矸石淋溶液主要污染组分总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2+))、钠(Na~+)在地下水系统中的多组分运移机理和污染规律:总硬度(Ca~(2+)+Mg~(2+))的运移速度很快,硫酸盐(SO_4~(2-))次之,而钠离子(Na~+)的运移速度最慢;对流、水动力弥散和吸附作用是造成总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))和钠离子(Na~+)运移的主要原因,对污染组分的运移起主要作用;土壤介质对总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))和钠离子(Na~+)都发生了吸附作用,且吸附强弱不同,对钠离子(Na~+)的吸附最强,硫酸盐(SO_4~(2-))次之,而对总硬度(Ca~(2+)+Mg~(2+))的吸附较弱,且土壤介质对三者的吸附都符合线性等温平衡吸附规律。并测定了土壤的渗透系数、水动力弥散系数以及总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠(Na~+)在饱水砂性土壤中的吸附分配系数(cm~3/g)和迟滞因子分别为1.59×10~(-2)cm~3/g、6.5×10~(-2)cm~3/g、4.22×10~(-1)cm~3/g和1.08、1.34、3.21,为模型的验证和数值模拟提供了可靠的实测参数;
(3)系统地分析了影响污染组分运移的主要因素,建立了综合考虑对流、水动力弥散、吸附解吸及存在源汇项条件下的定量描述土壤-地下水系统中主要污染组分运移三维动力学耦合数学模型,利用有限差分方法对数学模型进行了数值离散,给出了数值解法;
(4)利用数值模拟方法,对煤矸石淋溶液中主要污染组分总硬度(Ca~(2+)+Mg~(2+))、硫酸盐(SO_4~(2-))、钠离子(Na~+)在研究区域地下水系统中的浓度时空分布规律进行了三维数值模拟研究,结果表明:污染面积随时间推移不断向两轴方向扩大,且纵向显著,在地下水流的下方向,污染范围较大,地下水流的上方向,污染范围较小,地下水流的两侧方向,污染范围基本呈对称分布;污染组分浓度值向两轴方向逐次递减,淋溶液对地下水体污染程度与距污染源的距离有关,距离污染源越远,溶质的浓度越低;在垂向方向,污染组分随水流运移的同时逐渐向下方渗漏,污染面积不断扩大,并逐次递减,在污染源下部的0-20m深度范围内含量最高;而同一位置污染组分的浓度值随时间的延续呈逐渐增大的趋势,最后达到平衡;总硬度(Ca~(2+)+Mg~(2+))在地下水中运移的速度大于硫酸根的运移速度,更大于钠离子(Na~+)的运移速度;模拟相同时间后总硬度(Ca~(2+)+Mg~(2+))的运移范围较大,硫酸根(SO_4~(2-))的运移范围次之,而钠离子(Na~+)的运移范围最小,总硬度(Ca~(2+)+Mg~(2+))最先达到平衡,硫酸根(SO_4~(2-))次之,而钠离子(Na~+)的运移非常缓慢,所以总硬度(Ca~(2+)+Mg~(2+))、硫酸根(SO_4~(2-))污染的范围比钠离子(Na~+)污染的范围广,对地下水质破坏的程度比较严重;
(5)通过对新邱原南露天矿煤矸石山周围地区的地下水水质进行的调查、监测表明:该区地下水受到了严重污染,且污染源主要来自煤矸石山。煤矸石山是长期的污染源,是造成周围地区地下水无机盐类污染的主要原因。这一结论与波兰学者对380余座煤矸石山进行研究发现的煤矸石山是地下水污染的长期污染源以及煤矸石的主要污染是盐度、含硫量和潜在的酸性等基本是一致的;
(6)将数值模拟值与研究区域地下水多年的监测数据进行对比,进一步验证了所建数学模型的可靠性。该数学模型和数值模拟方法对其它地区煤矸石淋溶液对地下水系统污染问题普遍适用。
最后对煤矸石山淋溶液对地下水污染问题提出了治理措施。
本文的研究成果对于揭示煤矸石对地下水系统污染的环境动力学行为具有重要的科学理论意义,对地下水环境污染的预测、预报和管理具有重要的理论意义和实际意义,为更科学、更有效地预防、控制和治理矿区煤矸石固体废物排放带来的地下水系统污染问题提供了科学理论依据。
Based on the previous research results,the multi-disciplinary relevant theories of the groundwater dynamics,porous medium fluid dynamics, environmental chemistry and hydrogeology,and the combination of the theories, experiments and numerical simulation,this paper conducted a series of further investigations on pollution mechanism and laws of coal gangue leaching solution to groundwater system:
(1)The bench scale.soaking- leaching and dynamic leaching experiment indicates:the main pollution components released by the coal gangue of different rate of decay under water-rock interaction in Xinqiu open-cut mine are total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-)),sodium(Na~+)and total dissolved solid(TDS),the results of which are basically in accordance with the investigation of the 380 plus coal gangue hills in Poland conducted by Szcepanska;The coal gangue is eroded under geophysical function,chemical erosion and natural precipitation in the company of the oxidation, decomposition and dissolution reactions of the pyrite and the dissolution of the carbonate and aluminosilicate minerals.The higher the rate of decay is,the more pollution components the coal gangue releases;The main factors influencing the dissolution-release are the solid-liquid ratio,soak time,acidity, agitation,grain size and water dynamic flow.Moreover,heterogeneous reaction kinetics mechanism of the dissolution-release of the main pollution components was revealed,which abides by the Fick' s law;And builds the index fading equation of the dissolution-release regularity of the main pollution components and precipitation:C_v=C_0V~n,which can quantitatively predicts the pollution intensity of the main pollution components to groundwater system under atmospheric precipitation.
(2)The laboratory column dynamic simulating experiment reveals the multicomponent transport mechanism and pollution laws of the main pollution components of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+)in soil-groundwater system.That is,the transport velocity of the total hardness (Ca~(2+)+Mg~(2+))is the biggest followed by sulfate(SO_4~(2-)),and sodium(Na~+)the lowest.Namely,advection,mechanical dispersion and adsorption are the principal reasons of the transport of the total hardness(Ca~(2+)+Mg~(2+)), sulfate(SO_4~(2-))and sodium(Na~+)and play an vital role in the transport. Adsorption of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+) occurs in the soil medium,while the adsorption intensity is different.The adsorption of sodium(Na~+)is the strongest followed by sulfate(SO_4~(2-)),and total hardness(Ca~(2+)+Mg~(2+))the weakest.In general,their adsorption conforms to the linear equilibrium sorption isotherm.The soil conductivity,fluid dynamic dispersivity,adsorption distribution coefficient and retardation factor of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium(Na~+)are also measured.The adsorption distribution coefficient and retardation factor for the three are 1.59×10-2 cm~3/g、6.5×10-2cm~3/g、4.22×10-1 cm~3/gand1.08,1.34,3.21,these offer measured parameters for model verification and numerical simulation.
(3)Systematically analyze the essential factors influencing the pollution component transport and build three-dimensional dynamic coupled numerical model to describe the transport of the main pollution components in soil-groundwater system under the consideration of advection,hydrodynamic dispersion,adsorption-desorption and source and sink.The model underwent numerical discretization using finite-difference and the numerical solution was given.
(4)Numerical simulation.was conducted to the concentration temporal and spatial distribution of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-))and sodium (Na~+)in the groundwater system,the results of which indicate:The pollution area enlarges continuously with the passage of time and the longitudinal direction is more remarkable.The pollution scale is bigger in the groundwater downstream,smaller in the upstream,and distributes symmetrically on both sides;The pollutant concentration decreases gradually on either axis and the pollution degree of the leaching solution to the groundwater system is related to the distance of the pollution sources,the farther away from sources of pollution, the concentration of solute lower;In the vertical direction,with the current migration of contaminants at the same time gradually to the bottom of leaks, pollution area continued to expand,and successive decline.In the lower part of the pollution sources within 0-20m depth of the highest.The pollutant concentration in one location increases gradually with the passage of time and finally reaches equilibrium;The transport velocity of total hardness(Ca~(2+)+Mg~(2+)) is bigger than that of sulfate and much bigger than that of sodium;In the same simulation time period,the transport scale of total hardness(Ca~(2+)+Mg~(2+))is the largest and then sulfate(SO_4~(2-))and sodium(Na~+)sequentially.The total hardness(Ca~(2+)+Mg~(2+))comes to equilibrium first followed by sulfate(SO_4~(2-)) and sodium(Na~+)the slowest,so the pollution scale of hardness(Ca~(2+)+Mg~(2+)) and sulfate(SO_4~(2-))is larger than that of sodium(Na~+)and eventually causes more severe pollution to the groundwater.
(5)The investigation and monitoring to the water quality of groundwater in the surrounding areas of the coal gangue hills in formal Xinqiu open-cut mine demonstrate that the investigation areas have been polluted heavily by main pollution components of total hardness(Ca~(2+)+Mg~(2+)),sulfate(SO_4~(2-)),sodium(Na ~+)and total dissolved solid(TDS).The pollution sources is the coal gangue hill. The coal gangue hill is a long-term pollution source and is the main reason of groundwater inorganic salts pollution in the surrounding areas,which is also in accordance with the study conducted in Poland.
(6)The simulation results were compared with the many-year monitoring datas of the groundwater in the study region,which demonstrates that the mathematical model built is reliable.The model and numerical simulation method are also applicable to the pollution of inorganic salts to the groundwater in other regions.
In the end,the countermeasures were given to the groundwater pollution issues by coal gangue.
This study is of great scientific significance to reveal the environmental dynamics of the groundwater pollution by coal gangue.It is also of great theoretical and practical significance to predict,forecast and manage the groundwater pollution and lays theoretical foundations for preventing, controlling and treating the groundwater pollution issues caused by coal gangue in coal mine sites scientifically and efficiently.
引文
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