关中盆地地下环境氮污染机理与地下水质安全评价
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摘要
地下环境氮污染对生态环境安全和人体健康构成了潜在的危险,一直是环境和水文地质领域研究的热点和难点问题。本文以关中盆地为典型研究区,以包气带和浅层地下水为研究对象,以“三氮”的迁移转化为主线,以资料收集、原位试验、室内实验、理论分析和数值模拟为手段,开展了地下环境氮污染机理和水质安全评价研究,取得如下主要研究成果：
(1)研究区包气带和浅层地下水中“三氮”普遍存在,硝态氮的含量明显高于铵态氮和亚硝态氮的含量。在浅层地下水中硝态氮污染程度相对较重,呈面状分布,而铵态氮和亚硝态氮污染较轻,以点状存在。人类活动释放的氮负荷直接影响地下环境的氮污染程度,包气带岩性、厚度、地层结构和含水层的水力传输性能及其环境要素决定地下环境中“三氮”的存在形态和迁移转化规律。
(2)在系统分析氮化物行为特征的基础上,研究了铵态氮吸附/解吸的动力学过程。通过铵态氮等温吸附/解吸实验表明,黄土等温吸附/解吸方程符合Langmuir模型,解吸滞后性最强；粉质粘土和粉砂等温吸附/解吸模式符合Henry模型,解吸滞后性较强；而细砂等温吸附方程符合Langmuir模型,等温解吸模式符合Henry模型,解吸滞后性最弱。这些结论与前人的成果具有一致性,也充分表明了黄土包气带对铵态氮迁移的阻滞能力强,粉质粘土和粉砂包气带次之,细砂包气带的阻滞能力最弱。
(3)硝化/反硝化作用实验表明,铵态氮硝化动力学过程划分为缓慢阶段、快速阶段和衰减阶段,硝态氮反硝化过程包含反硝化阶段和弱硝化阶段,反硝化率为22.13%-70.23%,即在包气带原生环境(缺少人为添加营养液)中,硝态氮不能完全生物降解,使大部分硝态氮流失进入地下水中,为地下水硝态氮污染提供了物源。
(4)通过混合实验和密封浸泡实验初步证明,混合稀释作用并不降低硝态氮的总量；化学还原和生物反硝化是硝态氮总量减少的重要途径,其中以化学还原为主,生物反硝化为辅。硝态氮的自然转化率为25.7-39.9%,即含水层的自净能力较差,因此造成了硝态氮的积累。亚铁盐的添加强化了还原环境,使含水层中硝态氮的转化率提高2倍以上,这一研究可为地下水氮污染防治提供理论基础和技术支持。
(5)通过原位试验,对“三氮”在黄土和砂性包气带中迁移转化规律进行了对比研究。利用包气带水分和溶质运移模型,得出植物根系吸收作用明显降低氮化物的残留值和最大迁移距离；玉米根系吸收作用强于小麦根系,二者的吸氮量占施氮量的41.3%；通过黄土、粉砂和细砂包气带输入浅层地下水的氮化物以硝态氮为主,硝态氮通量为铵态氮和亚硝态氮通量的104倍以上。依据质量守恒定律,建立了含水层硝态氮年积累估算的数学模型,确定了影响硝态氮年积累的阈值,研究成果补充完善了含水层中氮化物环境行为与归趋理论。
(6)利用健康风险评价的理论和方法,开展了研究区浅层地下水氮污染健康风险评价,评价结果表明：浅层地下水中硝态氮对人体健康的慢性毒害指数较高,高风险区占研究区面积的78.2%,主要分布在农业活动强烈的灌区和人口居住密集、工业相对发达的城镇区；硝态氮含量在12.6-20mg/L间的地下水对人体健康也是高风险的,即传统意义上可以饮用的三类水对人体健康并不都是安全的。在重点城郊区(西安地区),开展了地下水质健康风险综合评价,指出硝态氮为地下水中应优先治理的物质。在此基础上,提出了基于健康风险的地下水质安全管理程序和保障措施,为地下水资源管理和保护提供了技术支持。
The nitride pollution has posed a potential danger on the ecological environment and human health, which is always a hot and difficult science problem in the study region of environmental science and hydrogeology. The nitride pollution mechanism and the safety of water quality in the vadose zone and shallow groundwater of the typical study area in Guanzhong Basin were studied. The data collection, in situ test, lab experimentations, numerical simulation and theoretical analysis were used to research the migration and transformation and fate of "three nitrogen". Through these works, some main research results were obtained, as follows:
(1) The "Three Nitrogen" exists generally in vadose zone and shallow groundwater in study region. The nitrate content was significantly higher than the content of ammonium nitrogen and nitrite. The nitrate presents the face-shaped pollution form in shallow groundwater, and the ammonium nitrogen and nitrite present point pollution form. The human activity is the excitation factor of nitrogen pollution in ground environment. The vadose zone lithology and thickness, stratum construction, the hydraulic condition of aquifer and environment factor are the critical factors of "Three Nitrogen" existence form and migration and transformation in ground environment.
(2) According to the systematic analysis of the nitride geochemical behavior, the ammonium nitrogen adsorption/desorption process was studied. The ammonium nitrogen adsorption/desorption experiments results show:The loess isothermal adsorption/desorption equations are consistent with Langmuir adsorption kinetics models, and the loess desorption hysteresis is the strongest. The silty clay and silt isothermal adsorption/desorption equations accords with the Henry model, and the silty clay and silt desorption hysteresis are stronger than fine sand. The fine sand isothermal adsorption equations is consistent with the Langmuir adsorption kinetics models and the isothermal desorption equations is consistent with Henry model, and the fine sand desorption hysteresis are the weakest. So, the loess vadose zone has the strongest hysteresis for the ammonium nitrogen, the silty clay and silt vadose zone has stronger hysteresis, but the fine sand vadose zone has the weakest hysteresis.
(3) The nitrification and denitrification experiments show:the ammonium nitrogen nitrification kinetics is divided into the slow phase, fast phase and decay phase (denitrification phase), and the nitrate denitrification process consist of the denitrification phase and the weak nitrification phase. The Nitrate denitrification rate is 22.13%-70.23%, which means the nitrate can not be completely biodegradable in the native soil environment (lack of man-added nutrient solution). So, the more nitrate go into the groundwater, which supply abundant substance for the nitride pollution of the groundwater.
(4) The mixture and sealed soak experiment approved that the mixture dilution cannot decrease the content of nitrate, and the chemical reduction and biological denitrification are the important paths to decrease the content of nitrate, that the nitrate natural degradation is dominated by chemical reduction, and supplemented by biological denitrification. The nitrate natural degradation rate is 25.7-39.9% in aquifer. The self-purification capacity of aquifer is bad and the nitrate is easy accumulating in the aquifer. The research proves the artificial strengthen chemical reduction (add the ferrous iron salt) is more than two times higher than the original ecological degradation. This study result can provide a theoretical basis and technical support for groundwater nitrogen pollution prevention and control.
(5) Through the in situ testing, the migration and transformation rule of "Three Nitrogen" in loess and sand vadose zone was studied. According to the vadose zone soil moisture and solute transport model, the plant root water uptake and nitrogen absorption reduces the residual value of nitride and maximum migration distance was studied. The corn root water uptake and nitrogen absorption was stronger than that of wheat roots, nitrogen absorption of wheat and corn root accounted for 41.3% of the total nitrogen. Nitrate flux, correspondingly through the loess, silt and fine sand vadose zone to the shallow groundwater, the nitrate is a difference of 104 times from the input flux of ammonium nitrogen and nitrite. A mathematical model based on conservation of mass is set up to estimate nitrate accumulation in the aquifer, and compute the threshold influencing the annual nitrate accumulation; The research complement the nitride environmental behavior and fate theory in aquifer.
(6) At last, the groundwater health risk assessment in study region was evaluated, the assessment results shows that the nitrate non-carcinogenic chronic toxic index for people health is higher in study region shallow groundwater. The high risk region is occupied 78.2% in study area, which distribute chiefly in the irrigation area and town with dense-residence, advanced-industry. The groundwater containing 12.6-20mg/L nitrate has high risk to people health. Through groundwater health risk assessment in Xi'an region, the author analysis put forward that the nitrate is the priority remediation matter. For, the safety management program and safeguard measures of underground water quality based on health risk, is proposed initially to put forward a new model for managing and protecting the groundwater resource.
(1)研究区包气带和浅层地下水中“三氮”普遍存在,硝态氮的含量明显高于铵态氮和亚硝态氮的含量。在浅层地下水中硝态氮污染程度相对较重,呈面状分布,而铵态氮和亚硝态氮污染较轻,以点状存在。人类活动释放的氮负荷直接影响地下环境的氮污染程度,包气带岩性、厚度、地层结构和含水层的水力传输性能及其环境要素决定地下环境中“三氮”的存在形态和迁移转化规律。
(2)在系统分析氮化物行为特征的基础上,研究了铵态氮吸附/解吸的动力学过程。通过铵态氮等温吸附/解吸实验表明,黄土等温吸附/解吸方程符合Langmuir模型,解吸滞后性最强；粉质粘土和粉砂等温吸附/解吸模式符合Henry模型,解吸滞后性较强；而细砂等温吸附方程符合Langmuir模型,等温解吸模式符合Henry模型,解吸滞后性最弱。这些结论与前人的成果具有一致性,也充分表明了黄土包气带对铵态氮迁移的阻滞能力强,粉质粘土和粉砂包气带次之,细砂包气带的阻滞能力最弱。
(3)硝化/反硝化作用实验表明,铵态氮硝化动力学过程划分为缓慢阶段、快速阶段和衰减阶段,硝态氮反硝化过程包含反硝化阶段和弱硝化阶段,反硝化率为22.13%-70.23%,即在包气带原生环境(缺少人为添加营养液)中,硝态氮不能完全生物降解,使大部分硝态氮流失进入地下水中,为地下水硝态氮污染提供了物源。
(4)通过混合实验和密封浸泡实验初步证明,混合稀释作用并不降低硝态氮的总量；化学还原和生物反硝化是硝态氮总量减少的重要途径,其中以化学还原为主,生物反硝化为辅。硝态氮的自然转化率为25.7-39.9%,即含水层的自净能力较差,因此造成了硝态氮的积累。亚铁盐的添加强化了还原环境,使含水层中硝态氮的转化率提高2倍以上,这一研究可为地下水氮污染防治提供理论基础和技术支持。
(5)通过原位试验,对“三氮”在黄土和砂性包气带中迁移转化规律进行了对比研究。利用包气带水分和溶质运移模型,得出植物根系吸收作用明显降低氮化物的残留值和最大迁移距离；玉米根系吸收作用强于小麦根系,二者的吸氮量占施氮量的41.3%；通过黄土、粉砂和细砂包气带输入浅层地下水的氮化物以硝态氮为主,硝态氮通量为铵态氮和亚硝态氮通量的104倍以上。依据质量守恒定律,建立了含水层硝态氮年积累估算的数学模型,确定了影响硝态氮年积累的阈值,研究成果补充完善了含水层中氮化物环境行为与归趋理论。
(6)利用健康风险评价的理论和方法,开展了研究区浅层地下水氮污染健康风险评价,评价结果表明：浅层地下水中硝态氮对人体健康的慢性毒害指数较高,高风险区占研究区面积的78.2%,主要分布在农业活动强烈的灌区和人口居住密集、工业相对发达的城镇区；硝态氮含量在12.6-20mg/L间的地下水对人体健康也是高风险的,即传统意义上可以饮用的三类水对人体健康并不都是安全的。在重点城郊区(西安地区),开展了地下水质健康风险综合评价,指出硝态氮为地下水中应优先治理的物质。在此基础上,提出了基于健康风险的地下水质安全管理程序和保障措施,为地下水资源管理和保护提供了技术支持。
The nitride pollution has posed a potential danger on the ecological environment and human health, which is always a hot and difficult science problem in the study region of environmental science and hydrogeology. The nitride pollution mechanism and the safety of water quality in the vadose zone and shallow groundwater of the typical study area in Guanzhong Basin were studied. The data collection, in situ test, lab experimentations, numerical simulation and theoretical analysis were used to research the migration and transformation and fate of "three nitrogen". Through these works, some main research results were obtained, as follows:
(1) The "Three Nitrogen" exists generally in vadose zone and shallow groundwater in study region. The nitrate content was significantly higher than the content of ammonium nitrogen and nitrite. The nitrate presents the face-shaped pollution form in shallow groundwater, and the ammonium nitrogen and nitrite present point pollution form. The human activity is the excitation factor of nitrogen pollution in ground environment. The vadose zone lithology and thickness, stratum construction, the hydraulic condition of aquifer and environment factor are the critical factors of "Three Nitrogen" existence form and migration and transformation in ground environment.
(2) According to the systematic analysis of the nitride geochemical behavior, the ammonium nitrogen adsorption/desorption process was studied. The ammonium nitrogen adsorption/desorption experiments results show:The loess isothermal adsorption/desorption equations are consistent with Langmuir adsorption kinetics models, and the loess desorption hysteresis is the strongest. The silty clay and silt isothermal adsorption/desorption equations accords with the Henry model, and the silty clay and silt desorption hysteresis are stronger than fine sand. The fine sand isothermal adsorption equations is consistent with the Langmuir adsorption kinetics models and the isothermal desorption equations is consistent with Henry model, and the fine sand desorption hysteresis are the weakest. So, the loess vadose zone has the strongest hysteresis for the ammonium nitrogen, the silty clay and silt vadose zone has stronger hysteresis, but the fine sand vadose zone has the weakest hysteresis.
(3) The nitrification and denitrification experiments show:the ammonium nitrogen nitrification kinetics is divided into the slow phase, fast phase and decay phase (denitrification phase), and the nitrate denitrification process consist of the denitrification phase and the weak nitrification phase. The Nitrate denitrification rate is 22.13%-70.23%, which means the nitrate can not be completely biodegradable in the native soil environment (lack of man-added nutrient solution). So, the more nitrate go into the groundwater, which supply abundant substance for the nitride pollution of the groundwater.
(4) The mixture and sealed soak experiment approved that the mixture dilution cannot decrease the content of nitrate, and the chemical reduction and biological denitrification are the important paths to decrease the content of nitrate, that the nitrate natural degradation is dominated by chemical reduction, and supplemented by biological denitrification. The nitrate natural degradation rate is 25.7-39.9% in aquifer. The self-purification capacity of aquifer is bad and the nitrate is easy accumulating in the aquifer. The research proves the artificial strengthen chemical reduction (add the ferrous iron salt) is more than two times higher than the original ecological degradation. This study result can provide a theoretical basis and technical support for groundwater nitrogen pollution prevention and control.
(5) Through the in situ testing, the migration and transformation rule of "Three Nitrogen" in loess and sand vadose zone was studied. According to the vadose zone soil moisture and solute transport model, the plant root water uptake and nitrogen absorption reduces the residual value of nitride and maximum migration distance was studied. The corn root water uptake and nitrogen absorption was stronger than that of wheat roots, nitrogen absorption of wheat and corn root accounted for 41.3% of the total nitrogen. Nitrate flux, correspondingly through the loess, silt and fine sand vadose zone to the shallow groundwater, the nitrate is a difference of 104 times from the input flux of ammonium nitrogen and nitrite. A mathematical model based on conservation of mass is set up to estimate nitrate accumulation in the aquifer, and compute the threshold influencing the annual nitrate accumulation; The research complement the nitride environmental behavior and fate theory in aquifer.
(6) At last, the groundwater health risk assessment in study region was evaluated, the assessment results shows that the nitrate non-carcinogenic chronic toxic index for people health is higher in study region shallow groundwater. The high risk region is occupied 78.2% in study area, which distribute chiefly in the irrigation area and town with dense-residence, advanced-industry. The groundwater containing 12.6-20mg/L nitrate has high risk to people health. Through groundwater health risk assessment in Xi'an region, the author analysis put forward that the nitrate is the priority remediation matter. For, the safety management program and safeguard measures of underground water quality based on health risk, is proposed initially to put forward a new model for managing and protecting the groundwater resource.
引文
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