Adsorption/Desorption Behavior of NH4-N under Surface Water-Groundwater Interaction and Its Impact on N Migration and Transformation
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摘要: 铵吸附/解吸是控制氮转化的重要反应之一，但其在地表水-地下水相互作用影响下对氮迁移转化的影响机制尚不清晰.以江汉平原东部沙湖监测场为研究区，通过分析地下水位及其水化学指标长期监测数据，结合室内土柱实验和反应迁移数值模型解译，识别了地表水补给和地下水排泄两种模式下NH4-N的迁移转化过程，探究了水动力驱动下N的迁移转化机制.研究表明，农业活动带来的高浓度NH4-N会被表层沉积物颗粒吸附；地表水入渗会促进沉积物中NH4-N的解吸附及后续的硝化作用，引起地下水中NO3-N浓度上升；含NH4-N的地下水排泄过程会促进沉积物对NH4-N的吸附，使沉积物中NH4-N吸附量升高.阳离子交换是影响NH4-N迁移转化的关键机制，地表水-地下水相互作用引起的水文地球化学环境变化影响了NH4-N的吸附/解吸及后续生物地球化学反应.Abstract: The migration and transformation of NH4-N are influenced by the interactions between surface water and groundwater. However, the mechanisms remain poorly understood. Continuous monitoring of the water level and its hydrochemical composition was conducted in the Shahu site. Column experiments and reactive transport modeling were applied to identify the migration and transformation of NH4-N under conditions of both surface water recharge and groundwater discharge. In this study it indicates that most injected NH4-N is adsorbed on shallow sediment. Infiltration of surface water enhances desorption of NH4-N from sediment particle and subsequent nitrification reactions. In contrast, adsorption of NH4-N on sediment is favored during discharge of NH4-N containing groundwater. Simulating results emphasize the crucial role of cation exchange in NH4-N mobility. Alterations in the hydrogeochemical environment during surface water-groundwater interactions impact the NH4-N adsorption/desorption behaviors and associated biogeochemical reactions.
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Key words:
- ammonium nitrogen /
- ion exchange /
- reactive transport modeling /
- surface water /
- groundwater /
- Jianghan Plain /
- hydrogeology
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图 4 研究区不同深度地下水化学指标季节性变化
Fig. 4. Seasonal variation of groundwater and surface water levels
图 5 地表水模拟液淋滤实验(a)和地下水模拟液淋滤实验(b) Br-的穿透曲线
符号表示观测值，实线表示计算值
Fig. 5. Breakthrough curve of Br- for synthetic surface water leaching experiment (a) and synthetic groundwater leaching experiment (b)
图 6 地表水模拟液淋滤实验(a)和地下水模拟液淋滤组实验(b)水化学成分变化
符号表示观测值，实线表示计算值
Fig. 6. Changes in water chemistry in synthetic surface water leaching experiment (a) and synthetic groundwater leaching group experiment (b)
图 7 地表水模拟液淋滤实验沉积物中吸附态离子含量变化
Fig. 7. Variation of adsorbed ions in sediments of synthetic surface water leaching experiment
图 8 地下水模拟液淋滤实验沉积物中吸附态离子含量变化
Fig. 8. Variation of adsorbed ions in sediments of synthetic groundwater leaching experiment
图 9 枯水期(a)与丰水期(b)氮素迁移转化的概念模型
Fig. 9. Conceptual model of nitrogen migration and transformation during periods of water depletion (a) and water abundance (b)
表 1 淋滤液水化学组成
Table 1. Chemical compositions of leachate water
组分 单位 灌溉水模拟液 地表水模拟液 地下水模拟液 NH4+ mmol/L 5.46 0.05 0.50 Ca2+ mmol/L 3.50 1.00 3.00 Mg2+ mmol/L 1.00 0.50 1.20 Na+ mmol/L 0.50 0.50 1.00 K+ mmol/L 1.00 0.10 0.05 Cl- mmol/L 8.00 2.30 8.40 SO42- mmol/L 0.50 0.35 0.00 NO3- mmol/L 0.00 0.15 0.00 Br- mmol/L 1.00 0.00 0.00 HCO3- mmol/L 6.00 0.50 1.55 pH 7.97 8.10 7.20 DO mmol/L 0.30 0.30 < 0.05 
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表 2 阳离子交换反应方程式和对应的热力学参数(Parkhurst and Appelo, 2013)
Table 2. Cation exchange reaction equations and corresponding thermodynamic parameters
反应 K Ca2+ + 2NH4X = CaX2 + 2NH4+ 0.4 Mg2+ + 2NH4X = MgX2 + 2NH4+ 0.25 Na+ + NH4X = NaX + NH4+ 0.25 K+ + NH4X = KX + NH4+ 1.26
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表 3 Monod方程参数(Prommer et al., 2006)
Table 3. Parameters of the Monod equation
反应参数 单位 值 $ {k}_{\mathrm{m}\mathrm{a}\mathrm{x}\_\mathrm{N}{\mathrm{H}}_{4}^{+}} $ mol/(L·s) 8×10-10 $ {k}_{\mathrm{m}\mathrm{N}{\mathrm{H}}_{4}^{+}} $ mol/L 1×10-4 $ {k}_{\mathrm{m}{\mathrm{O}}_{2}} $ mol/L 1.5×10-5
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表 4 对流-弥散方程及其他计算参数
Table 4. Parameters related of the convection-dispersion equation and computational parameters
实验组 达西流速(m/s) 有效孔隙度 弥散度(m) 弥散系数 地表水模拟液淋滤实验 0.12 0.46 0.000 1 4×10-9 地下水模拟液淋滤实验 0.12 0.47 0.000 1 4×10-9
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