Co-Migration and Transformation Mechanism of Dissolved Iron and Arsenic during Groundwater Discharge into River Water
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摘要: 地下水排泄河水过程中会将缺氧地下水中的Fe2+与As3+带入含氧的交互带中，本研究旨在探明该过程中Fe2+与As3+随地下水在实际沉积物介质中的协同迁移转化机制.通过室内柱实验和批实验研究地下水排泄河水时Fe2+、As3+的迁移转化规律并获取其在交互带不同部位向固相转化（固化）的速率.结果表明：沉积物对Fe2+、As3+具有较强的吸附作用，As3+加快了Fe2+的迁移；Fe2+在流经交互带时发生化学氧化沉淀，形成了Fe-As结合态矿物.从远河处至近河处河处，Fe2+、As3+的固化速率加快.在整个交互带区域Fe2+明显促进了As3+的固化，在离河较近的区域As3+略微抑制了Fe2+的固化.地下水排泄河水过程中，Fe2+、As3+在交互不同部位以不同的速率发生协同化学氧化和吸附固定，从而严重阻碍其向河水方向迁移.Abstract: During groundwater discharge into the river, Fe2+ and As3+ in anoxic groundwater are brought into the oxygen-containing interaction zone. This study explores the co-migration and transformation mechanism of Fe2+ and As3+with groundwater in the natural sediment medium.The migration and transformation rules of Fe2+ and As3+during groundwater discharge into river water and the transformation rate of Fe2+ and As3+ to solid phase (solidification) in different regions of the interaction zone are studied by laboratory column experiment and batch experiment.The results show that the sediment strongly adsorbs Fe2+ and As3+, and As3+ accelerates the migration of Fe2+. The chemical oxidation and precipitation of Fe2+ occur, and Fe-As bounding minerals are formed when it flows through the interaction zone.The solidification rate of Fe2+ and As3+ is accelerated from the area far from the river to that near the river. In the whole interaction zone, Fe2+ significantly promotes the solidification of As3+, while As3+ slightly inhibits the solidification of Fe2+ near the river bank.In short, during groundwater discharge into river water, the synergistic chemical oxidation and adsorption fixation of Fe2+ and As3+in groundwater occur at different rates in different regions of the interaction zone, which seriously hinders their migration to river water.
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Key words:
- groundwater discharge /
- interaction zone /
- iron /
- arsenic /
- migration /
- hydrogeology
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图 1 地下水排泄过程中Fe2+、As3+迁移规律
Fe2+、As3+的单位为mM
Fig. 1. Migration of Fe2+ and As3+during groundwater discharge intoriverwater
图 2 柱中不同部位沉积的Fe(Ⅱ)、Fe(Ⅲ) 和各形态As含量
Fig. 2. Contents of secondary Fe(Ⅱ)、Fe(Ⅲ), and each form of As in different parts of the column
图 3 交互带不同部位孔隙水Fe2+、As3+消减曲线
R表示河水比例，Fe2+、As3+单位为mM；图a、c为单独的Fe2+和As3+的消减曲线；图b、d为Fe2+和As3+共存时Fe2+和As3+的消减曲线
Fig. 3. Reduction curves of Fe2+ and As3+ in pore water in different parts of interaction zone
图 4 交互带不同部位孔隙水Fe2+、As3+固化过程一级动力学拟合结果
R表示河水比例，Fe2+、As3+单位为mM
Fig. 4. First-order kinetic fitting results of Fe2+ and As3+ solidification processes in pore water in different parts of the interaction zone
图 5 交互带不同部位孔隙水Fe2+、As3+固化过程一级反应速率常数k变化趋势
Fig. 5. Variation trend of first-order reaction rate constant k during Fe2+ and As3+ solidification of pore water in different parts of the interaction zone
表 1 供试沉积物理化指标
Table 1. Ion content in the sediments tested
理化指标 单位 含量 理化指标 单位 含量 CEC cmol/kg 11.69 含水率 % 18.63 pH - 8.03 TOC % 10.13 Fe mg/g 13.12 As mg/g 0.01 Ca mg/g 10.13 Mn mg/g 0.53 Mg mg/g 0.78 Al mg/g 2.23 K mg/g 14.52 Na mg/g 13.12 Ba mg/g 0.37 Si mg/g 105.19 
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表 2 批次实验设计
Table 2. Batch experimental design
实验组 河水比例（%） Fe2+浓度（mM/L） As3+浓度（mM/L） 1 10 0.45 0 2 30 0.35 0 3 50 0.25 0 4 70 0.15 0 5 90 0.05 0 6 10 0 0.009 7 30 0 0.007 8 50 0 0.005 9 70 0 0.003 10 90 0 0.001 11 10 0.45 0.009 12 30 0.35 0.007 13 50 0.25 0.005 14 70 0.15 0.003 15 90 0.05 0.001
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表 3 交互带不同部位孔隙水Fe2+、As3+固化过程一级动力学拟合方程显著性检验参数
Table 3. Significance test parameters of first-order kinetic fitting results of Fe2+ and As3+ solidification processes in pore water in different parts of the interaction zone
实验组 河水比例（%） Fe2+浓度（mM/L） As3+浓度（mM/L） Fe2+拟合显著性检验参数R2 As3+拟合显著性检验参数R2 1 10 0.45 0 0.918 0 - 2 30 0.35 0 0.943 4 - 3 50 0.25 0 0.873 8 - 4 70 0.15 0 0.836 5 - 5 90 0.05 0 0.871 5 - 6 10 0 0.009 - 0.890 2 7 30 0 0.007 - 0.902 7 8 50 0 0.005 - 0.891 8 9 70 0 0.003 - 0.949 5 10 90 0 0.001 - 0.931 4 11 10 0.45 0.009 0.872 4 0.889 3 12 30 0.35 0.007 0.847 5 0.965 2 13 50 0.25 0.005 0.873 5 0.962 5 14 70 0.15 0.003 0.849 0 0.832 3 15 90 0.05 0.001 0.890 0 0.858 1
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