三峡库区典型区域氮、磷和农药非点源污染物随水文过程的迁移转化及其归趋研究
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摘要
三峡水库蓄水后，库区大部分次级河流回水区“水华”现象频发。农业生产使用的化肥、农药是破坏库区次级河流水质的主要原因，农村人畜粪便、生活污水和生活垃圾也是造成库区次级河流污染的重要原因。据不完全统计，三峡库区次级河流中总磷、总氮、有机物等污染物有52%~59%来自农业面源污染，三峡库区氮、磷和农药面源污染已成为威胁库区地表水和地下水污染最为严重的生态环境问题之一。因此，开展对三峡库区典型区域氮、磷和农药非点源污染迁移转化和时空分布规律的研究，对于三峡库区社会、经济和环境的可持续发展、促进库区生态和谐以及保障库区水环境安全具有重要的理论意义和实践价值。
本研究根据三峡库区气候、地形、地质、地貌、土地利用类型和紫色土坡地壤中流极为发育等特点，分别构建基于地表径流和壤中流的分布式溶解态非点源氮磷污染模型、基于不确定性理论的分布式吸附态氮磷污染灰色模型、和根据面源污染产生的动力学机制构建农药非点源污染综合迁移转化模型，并利用研究区水质实测数据进行模型验证。分别以三峡库区小江流域和忠县石宝镇新政村柑橘果园与菜地为例模拟库区典型区域总氮、总磷和农药面源污染物随水文过程的迁移转化和时空分布规律，并对污染负荷来源的关键源区进行识别，对流域氮、磷和农药面源污染的环境影响进行分析和评价。形成了较为完整的非点源污染耦合模型，实现了氮、磷和农药非点源污染的综合模拟。主要研究成果如下：
①考虑到壤中流产生的氮、磷非点源污染，引入具有物理机制的、以流域土地利用类型为研究单元的SLURP分布式水文模型，构建基于地表径流和壤中流的分布式溶解态非点源污染模型。通过参数的校准和优化，2003~2008年径流量模拟值与实测值的相对误差在20%以内，Nash-Sutcliffe系数为0.8左右，改善了地表径流量和壤中流量的模拟精度，提高了溶解态非点源氮磷污染负荷估算的准确性。
②鉴于降雨侵蚀因子和泥沙输移比因子的时空变化，建立能反映流域输沙量逐年变化的动态模型。结合通用土壤流失方程中各因子具有不确定性的特点，运用不确定性理论把各因子定义为盲因子，由土壤表层氮磷含量和污染物泥沙富集系数构建基于不确定性理论的分布式吸附态氮磷污染灰色动态模型，实现了GIS技术、不确定性理论和吸附态非点源污染模型的动态耦合。
③为了准确模拟流域输沙量，以与泥沙输移比密切相关的泥沙搬运力为切入点，以数字流域像元内和上游来水形成的累积径流量为突破口，根据累积径流量和泥沙搬运力的数学关系，把累积径流量分别与地形指数和流水累积量耦合，且假定具有最大泥沙搬运力像元的泥沙输移比为1，提出基于GIS空间分析技术的流域坡面和河道泥沙输移比新计算方法。为流域尺度土壤流失量的准确估算提供了科学的理论依据。
④污染物在植物冠层和土壤亚环境系统中的迁移机理有本质的不同，前者主要是植物冠层区农药的挥发，动力主要是蒸发，对应的方程为一阶微分方程；后者主要是农药在大气、水和土壤环境中的降解，动力主要是水势梯度和浓度梯度，对应的方程为二阶偏微分方程。根据污染物在不同媒质中迁移转化的动力学机制构建农药非点源污染综合迁移转化模型，用来描述气、水和土壤环境中农药污染物迁移转化的时空分布规律与输出过程。
⑤把流域氮、磷和农药非点源污染模型进行耦合，构建具有物理机制的、分布式的流域非点源污染综合动态模型，来模拟氮、磷和农药面源污染的时空分布特征和污染物输出量，进而对非点源污染负荷进行定量估算与分析评估。将更有利于准确全面地定量分析和评估三峡库区典型区域非点源污染负荷的动态变化规律，实现了农业氮、磷和农药非点源污染的综合模拟。
⑥论文以三峡库区小江流域和忠县石宝镇新政村农业用地为研究对象，在GIS技术支持下，借助构建的分布式综合模型，分别对氮、磷和农药非点源污染迁移转化及其趋向过程进行动态模拟验证。验证结果表明，模型构建方法合理，模拟效果良好。并据此对研究区非点源污染负荷的时空分布规律、来源构成、贡献率、关键源区、径流和侵蚀输出分别进行分析和评估。就年均情况而言，小江流域总氮负荷的来源贡献率大小依次为化肥施用（64.01%）＞水土流失（26.48%）＞畜禽养殖（5.14%）＞生活污染（4.37%），总磷负荷的来源贡献率大小依次为化肥施用（68.2%）＞水土流失（28.22%）＞畜禽养殖（2.64%）＞生活污染（0.94%）；三峡库区地表水体和表层土壤农药残留浓度水平取决于降雨强度、降雨历时，降雨量、径流量、农药施用和农田灌溉状况。
After impoundment of Three Gorges Reservoir, the hydrodynamic situation of therelated rivers in the reservoir area had undergone fundamental changes, abnormalproliferation phenomenon of “algae bloom” in tributaries continuously breaks out. Thechemical fertilizers and pesticides in the agricultural production are the main reasons forthe destruction of water quality in tributaries; rural human and animal feces, sewage andgarbage are also the important reasons for the pollution of tributaries in the reservoirarea. According to incomplete statistics,52%-59%of total phosphorus (TP), totalnitrogen (TN) and organic pollutants in the secondary rivers of the Three GorgesReservoir Area are from agricultural non-point source pollution. Nitrogen, phosphorusand pesticide non-point source pollution in Three Gorges Reservoir Area has becomeone of the most serious ecological problems for the contamination threat of surfacewater and groundwater in the reservoir area. Therefore, the study of migration andtransformation of nitrogen, phosphorus and pesticide non-point source pollution in atypical area of the Three Gorges Reservoir Area has important theoretical significancesand practical values for the social, economic and environmental sustainability of theThree Gorges Reservoir Area, and for the promotion of ecological harmony and theprotection of the water environment security in the reservoir area.
In this study, according to the characteristics of climate, topography, geology,geomorphology, land use types and well developed interflow in purple soil in ThreeGorges reservoir area, a distributed-dissolved non-point source nitrogen and phosphoruspollution model based on surface flow and interflow, a distributed-absorbed non-pointsource nitrogen and phosphorus pollution gray model based on the uncertainty theory,and a comprehensive migration and transformation model of pesticide pollution basedon the kinetic mechanism of non-point source pollution were built respectively, and thecalibration and validation of the model were carried out by observed data of runoff,sediment, and water quality from basin outlet. The Xiaojiang River basin, orchards andvegetable plots of Xinzheng village in Shibao Town, located in the hinterland of ThreeGorges Reservoir area, were chosen as typical case study area in this paper to simulatemigration and transformation, and spatial and temporal distribution of TN, TP, andpesticide non-point source pollutants with the hydrological processes. The criticalsource areas of pollution load were identified and the environmental impacts of nitrogen, phosphorus and pesticide non-point source pollution were analyzed and assessed,respectively. Therefore, the non-point source pollution coupled model was built toachieve the comprehensive simulation of nitrogen, phosphorus and pesticide non-pointsource pollution. The main findings are as follows:
①Taking into account nitrogen, phosphorus non-point source pollution of thesubsurface flow, the SLURP hydrological model with the physical mechanisms wasintroduced and assisted to build distributed-dissolved non-point source pollution modelbased on surface runoff and subsurface flow. Through calibration and optimization ofthe parameters, the simulation accuracy of the surface runoff and subsurface flow, andthe estimation accuracy of the dissolved non-point source nitrogen and phosphorusloading were both improved.
②In view of temporal and spatial variations of the rainfall erosion factor andsediment delivery ratio factor, the dynamic model which can reflect the annualvariations of the watershed sediment load was established. According to the uncertaintycharacteristics for each factor in the universal soil loss equation, each factor in theequation was defined as the blind factor, the distributed-adsorbed nitrogen andphosphorus pollution gray model was built via nitrogen and phosphorus content, andcontaminants enrichment efficiency. Overall, the dynamic coupling among the GIStechnology, uncertainty theory and adsorbed non-point source pollution model wasachieved successfully.
③In order to simulate watershed sedimenttransport accurately, the sedimenttransport capacity, which is closely related to sediment delivery ratio, was chosen as thestarting point, and the cumulative runoff amount from a pixel and the upper reaches ofthis pixel was selected as a key breakthrough. According to the mathematicalrelationship between sediment transport capacity and the cumulative runoff, thetopographic index and the flow accumulation were coupled with the cumulative runoff,and the sediment delivery ratio of the pixel with maximum sediment transport capacitywas assumed as1, a new calculation method of watershed slope and river channelsediment delivery ratio was proposed by means of the GIS spatial analysis techniques.This could provide scientific theory basis for the accurate estimation of the basin-scalesoil loss.
④The migration mechanism of pollutants in the plant canopy is essentiallydifferent from soil sub-environment system, the former is pesticides volatile from plantcanopy, the driving force is evaporation, and the corresponding equation is the first order differential equation; the latter is mainly the degradation of pesticides in the air,water and soil environment, the main driving force is the water potential gradient andconcentration gradient, and the corresponding equation is the second order partialdifferential equations. A comprehensive migration and transformation model ofpesticide non-point source pollution was built on the basis of dynamic mechanism ofpollutants migration and transformation in different media, and used to describe thespatial and temporal distribution and output process of pesticide pollutants in the air,water and soil environment.
⑤An integrated dynamic basin model, with physical and distributed mechanism,was built by coupling nitrogen, phosphorus and pesticide non-point source pollutionmodel to simulate pollution source strength of nitrogen, phosphorus and pesticidenon-point source pollution, and thus to quantitatively evaluate and analysis the temporaland spatial distribution of non-point source pollution load. This will be more accuratelyand comprehensively conducive to quantitatively analysis and evaluate the dynamicvariations of non-point source pollution load in a typical area of the Three Gorgesreservoir area, and will achieve a comprehensive simulation of the agricultural nitrogen,phosphorus and pesticide non-point source pollution.
⑥The Xiaojiang River watershed and the agricultural land in Xinzheng village,Shibao Town, Zhongxian in the Three Gorges Reservoir Area were selected as the casestudy of non-point source pollution, according to the established comprehensive model,the fate, migration and transformation of non-point source pollution of nitrogen,phosphorus and pesticides were simulated dynamically in support of GIS technology.The verifcation results show that the construction method of the model is reasonable.Based on this, the spatial and temporal distribution, the source composition, thecontribution rate, the critical source areas, runoff and erosion output of non-point sourcepollution load were analyzed and evaluated, respectively.
本研究根据三峡库区气候、地形、地质、地貌、土地利用类型和紫色土坡地壤中流极为发育等特点，分别构建基于地表径流和壤中流的分布式溶解态非点源氮磷污染模型、基于不确定性理论的分布式吸附态氮磷污染灰色模型、和根据面源污染产生的动力学机制构建农药非点源污染综合迁移转化模型，并利用研究区水质实测数据进行模型验证。分别以三峡库区小江流域和忠县石宝镇新政村柑橘果园与菜地为例模拟库区典型区域总氮、总磷和农药面源污染物随水文过程的迁移转化和时空分布规律，并对污染负荷来源的关键源区进行识别，对流域氮、磷和农药面源污染的环境影响进行分析和评价。形成了较为完整的非点源污染耦合模型，实现了氮、磷和农药非点源污染的综合模拟。主要研究成果如下：
①考虑到壤中流产生的氮、磷非点源污染，引入具有物理机制的、以流域土地利用类型为研究单元的SLURP分布式水文模型，构建基于地表径流和壤中流的分布式溶解态非点源污染模型。通过参数的校准和优化，2003~2008年径流量模拟值与实测值的相对误差在20%以内，Nash-Sutcliffe系数为0.8左右，改善了地表径流量和壤中流量的模拟精度，提高了溶解态非点源氮磷污染负荷估算的准确性。
②鉴于降雨侵蚀因子和泥沙输移比因子的时空变化，建立能反映流域输沙量逐年变化的动态模型。结合通用土壤流失方程中各因子具有不确定性的特点，运用不确定性理论把各因子定义为盲因子，由土壤表层氮磷含量和污染物泥沙富集系数构建基于不确定性理论的分布式吸附态氮磷污染灰色动态模型，实现了GIS技术、不确定性理论和吸附态非点源污染模型的动态耦合。
③为了准确模拟流域输沙量，以与泥沙输移比密切相关的泥沙搬运力为切入点，以数字流域像元内和上游来水形成的累积径流量为突破口，根据累积径流量和泥沙搬运力的数学关系，把累积径流量分别与地形指数和流水累积量耦合，且假定具有最大泥沙搬运力像元的泥沙输移比为1，提出基于GIS空间分析技术的流域坡面和河道泥沙输移比新计算方法。为流域尺度土壤流失量的准确估算提供了科学的理论依据。
④污染物在植物冠层和土壤亚环境系统中的迁移机理有本质的不同，前者主要是植物冠层区农药的挥发，动力主要是蒸发，对应的方程为一阶微分方程；后者主要是农药在大气、水和土壤环境中的降解，动力主要是水势梯度和浓度梯度，对应的方程为二阶偏微分方程。根据污染物在不同媒质中迁移转化的动力学机制构建农药非点源污染综合迁移转化模型，用来描述气、水和土壤环境中农药污染物迁移转化的时空分布规律与输出过程。
⑤把流域氮、磷和农药非点源污染模型进行耦合，构建具有物理机制的、分布式的流域非点源污染综合动态模型，来模拟氮、磷和农药面源污染的时空分布特征和污染物输出量，进而对非点源污染负荷进行定量估算与分析评估。将更有利于准确全面地定量分析和评估三峡库区典型区域非点源污染负荷的动态变化规律，实现了农业氮、磷和农药非点源污染的综合模拟。
⑥论文以三峡库区小江流域和忠县石宝镇新政村农业用地为研究对象，在GIS技术支持下，借助构建的分布式综合模型，分别对氮、磷和农药非点源污染迁移转化及其趋向过程进行动态模拟验证。验证结果表明，模型构建方法合理，模拟效果良好。并据此对研究区非点源污染负荷的时空分布规律、来源构成、贡献率、关键源区、径流和侵蚀输出分别进行分析和评估。就年均情况而言，小江流域总氮负荷的来源贡献率大小依次为化肥施用（64.01%）＞水土流失（26.48%）＞畜禽养殖（5.14%）＞生活污染（4.37%），总磷负荷的来源贡献率大小依次为化肥施用（68.2%）＞水土流失（28.22%）＞畜禽养殖（2.64%）＞生活污染（0.94%）；三峡库区地表水体和表层土壤农药残留浓度水平取决于降雨强度、降雨历时，降雨量、径流量、农药施用和农田灌溉状况。
After impoundment of Three Gorges Reservoir, the hydrodynamic situation of therelated rivers in the reservoir area had undergone fundamental changes, abnormalproliferation phenomenon of “algae bloom” in tributaries continuously breaks out. Thechemical fertilizers and pesticides in the agricultural production are the main reasons forthe destruction of water quality in tributaries; rural human and animal feces, sewage andgarbage are also the important reasons for the pollution of tributaries in the reservoirarea. According to incomplete statistics,52%-59%of total phosphorus (TP), totalnitrogen (TN) and organic pollutants in the secondary rivers of the Three GorgesReservoir Area are from agricultural non-point source pollution. Nitrogen, phosphorusand pesticide non-point source pollution in Three Gorges Reservoir Area has becomeone of the most serious ecological problems for the contamination threat of surfacewater and groundwater in the reservoir area. Therefore, the study of migration andtransformation of nitrogen, phosphorus and pesticide non-point source pollution in atypical area of the Three Gorges Reservoir Area has important theoretical significancesand practical values for the social, economic and environmental sustainability of theThree Gorges Reservoir Area, and for the promotion of ecological harmony and theprotection of the water environment security in the reservoir area.
In this study, according to the characteristics of climate, topography, geology,geomorphology, land use types and well developed interflow in purple soil in ThreeGorges reservoir area, a distributed-dissolved non-point source nitrogen and phosphoruspollution model based on surface flow and interflow, a distributed-absorbed non-pointsource nitrogen and phosphorus pollution gray model based on the uncertainty theory,and a comprehensive migration and transformation model of pesticide pollution basedon the kinetic mechanism of non-point source pollution were built respectively, and thecalibration and validation of the model were carried out by observed data of runoff,sediment, and water quality from basin outlet. The Xiaojiang River basin, orchards andvegetable plots of Xinzheng village in Shibao Town, located in the hinterland of ThreeGorges Reservoir area, were chosen as typical case study area in this paper to simulatemigration and transformation, and spatial and temporal distribution of TN, TP, andpesticide non-point source pollutants with the hydrological processes. The criticalsource areas of pollution load were identified and the environmental impacts of nitrogen, phosphorus and pesticide non-point source pollution were analyzed and assessed,respectively. Therefore, the non-point source pollution coupled model was built toachieve the comprehensive simulation of nitrogen, phosphorus and pesticide non-pointsource pollution. The main findings are as follows:
①Taking into account nitrogen, phosphorus non-point source pollution of thesubsurface flow, the SLURP hydrological model with the physical mechanisms wasintroduced and assisted to build distributed-dissolved non-point source pollution modelbased on surface runoff and subsurface flow. Through calibration and optimization ofthe parameters, the simulation accuracy of the surface runoff and subsurface flow, andthe estimation accuracy of the dissolved non-point source nitrogen and phosphorusloading were both improved.
②In view of temporal and spatial variations of the rainfall erosion factor andsediment delivery ratio factor, the dynamic model which can reflect the annualvariations of the watershed sediment load was established. According to the uncertaintycharacteristics for each factor in the universal soil loss equation, each factor in theequation was defined as the blind factor, the distributed-adsorbed nitrogen andphosphorus pollution gray model was built via nitrogen and phosphorus content, andcontaminants enrichment efficiency. Overall, the dynamic coupling among the GIStechnology, uncertainty theory and adsorbed non-point source pollution model wasachieved successfully.
③In order to simulate watershed sedimenttransport accurately, the sedimenttransport capacity, which is closely related to sediment delivery ratio, was chosen as thestarting point, and the cumulative runoff amount from a pixel and the upper reaches ofthis pixel was selected as a key breakthrough. According to the mathematicalrelationship between sediment transport capacity and the cumulative runoff, thetopographic index and the flow accumulation were coupled with the cumulative runoff,and the sediment delivery ratio of the pixel with maximum sediment transport capacitywas assumed as1, a new calculation method of watershed slope and river channelsediment delivery ratio was proposed by means of the GIS spatial analysis techniques.This could provide scientific theory basis for the accurate estimation of the basin-scalesoil loss.
④The migration mechanism of pollutants in the plant canopy is essentiallydifferent from soil sub-environment system, the former is pesticides volatile from plantcanopy, the driving force is evaporation, and the corresponding equation is the first order differential equation; the latter is mainly the degradation of pesticides in the air,water and soil environment, the main driving force is the water potential gradient andconcentration gradient, and the corresponding equation is the second order partialdifferential equations. A comprehensive migration and transformation model ofpesticide non-point source pollution was built on the basis of dynamic mechanism ofpollutants migration and transformation in different media, and used to describe thespatial and temporal distribution and output process of pesticide pollutants in the air,water and soil environment.
⑤An integrated dynamic basin model, with physical and distributed mechanism,was built by coupling nitrogen, phosphorus and pesticide non-point source pollutionmodel to simulate pollution source strength of nitrogen, phosphorus and pesticidenon-point source pollution, and thus to quantitatively evaluate and analysis the temporaland spatial distribution of non-point source pollution load. This will be more accuratelyand comprehensively conducive to quantitatively analysis and evaluate the dynamicvariations of non-point source pollution load in a typical area of the Three Gorgesreservoir area, and will achieve a comprehensive simulation of the agricultural nitrogen,phosphorus and pesticide non-point source pollution.
⑥The Xiaojiang River watershed and the agricultural land in Xinzheng village,Shibao Town, Zhongxian in the Three Gorges Reservoir Area were selected as the casestudy of non-point source pollution, according to the established comprehensive model,the fate, migration and transformation of non-point source pollution of nitrogen,phosphorus and pesticides were simulated dynamically in support of GIS technology.The verifcation results show that the construction method of the model is reasonable.Based on this, the spatial and temporal distribution, the source composition, thecontribution rate, the critical source areas, runoff and erosion output of non-point sourcepollution load were analyzed and evaluated, respectively.
引文
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