Effect of Nitrogen Cycling on Arsenic Release in Groundwater with High Arsenic Content
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摘要: 高As地下水中往往伴随着高NH4+组分的分布，但是有关氮循环如何影响As迁移释放的研究还较少.江汉平原为高砷地下水分布区，同时地下水中NH4+浓度也普遍较高，本研究旨在探讨江汉平原地下水系统中氮迁移转化对砷组分时空分布的控制过程.对江汉平原不同水体的水化学和同位素指标进行测试，利用氮和砷相关物理化学指标对采样点进行层次聚类分析.结果表明，沿着地下水流方向，由于地下水氧化还原环境等因素的改变，氮反应迁移过程对As释放过程的影响机制也不相同.在补给区附近，地下水处于偏氧化环境，NO3‒的富集会抑制铁氧化物溶解过程；沿地下水径流方向，地下水环境向还原条件转化，反硝化作用加强，促进了铁氧化物的溶解并导致As释放到地下水中；在地下水排泄区，地下水环境处于还原状态，反硝化反应进一步增强，可能发生利用Fe2+作为电子供体进行的反硝化反应和DNRA过程，进而通过氧化还原反应影响As释放.Abstract: Groundwater with high As concentration often contains high NH4+ components,but few studies have been conducted to investigate the effect of nitrogen cycling on the migration and release of As. The aquifer system in Jianghan Plain contains high arsenic as well as high content of ammonium in groundwater. The purpose of this study is to explore the effect of nitrogen reactive transport on the As release. In this study,the different water bodies in Jianghan Plain were sampled and their hydrochemical and isotopic indexes were tested,and hierarchical cluster analysis was performed on the sampling sites using the physicochemical indexes related to nitrogen and arsenic. The results show that along the direction of groundwater flow,due to the changes of groundwater redox conditions,the effect of nitrogen redox process on arsenic release process is different. Near the groundwater recharge area,the enrichment of NO3‒ in the relatively oxidized zone inhibits the dissolution of iron oxide. Along the groundwater flow path,the redox environment of aquifer system changes from oxidized to reduced condition. The enhanced denitrification occurring in the reduced environment could promote the dissolution of iron oxide,resulting in the release of As into groundwater. The denitrification is further enhanced in the groundwater discharge zone,and denitrification and DNRA using Fe2+ as electron donor may influence arsenic release.
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Key words:
- high arsenic groundwater /
- nitrogen /
- cluster analysis /
- Jianghan Plain /
- environmental geology /
- hydrogeology
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图 1 江汉平原地下水采样点分布
Fig. 1. Distribution map of groundwater sampling points in Jianghan Plain
图 8 δ15N-NO3‒，δ18O-NO3‒关系(据Liang et al., 2020)
Fig. 8. Relationship of δ15N-NO3‒ and δ18O-NO3‒ (after Liang et al., 2020)
图 9 δ15N-NO3‒，δ15N-NH4+垂向关系
Fig. 9. Vertical relationship of δ15N - NO3‒ and δ15N-NH4+
图 10 T_As和相关化学组分垂向分布
Fig. 10. Vertical distribution of related chemical composition and T_As
表 1 水样测试手段及方法
Table 1. Testing means and methods for water samples
测试指标 仪器或方法 最低检出浓度 测试单位 F‒、Cl‒、NO3‒、
SO42‒离子色谱法
(Dionex 2500，Thermo，美国)0.02、0.13、0.02、0.14 mg/L 中国地质大学(武汉)环境学院实验中心 Ca2+、Mg2+、
Na+、K+电感耦合等离子体发射光谱仪
(ICP-OES)0.003、0.020、0.020、0.150 μg/mL As 原子荧光分光光度计
(AFS-8220，北京吉天，中国)0.3 μg/L DOC 总有机碳分析仪
(multi N/C 3100，Elementar，德国)4 μg/L δ15N-NO3‒、
δ18O-NO3‒同位素比质谱仪
(Tracegas-lsoprime100，德国)0.2‰、0.7‰ 中国农业科学院环境稳定同位素实验室 δ15N-NH4+ 同位素比质谱仪(EA-lsoprime100, 德国) 0.2‰ 
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