Spatial-Temporal Distribution of Arsenic in Groundwater System in Tian-E-Zhou Wetland of the Yangtze River and Its Controlling Mechanism
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摘要: 高砷地下水不仅直接危害供水安全，还可通过与湿地之间的交互作用，影响湿地水质进而威胁湿地生态安全.长江中游河湖平原已被报道广泛分布有高砷地下水，而位于长江中游故道区域的天鹅洲湿地地下水中砷的空间分布特征尚不明确，湿地与地下水的交互作用对地下水中砷季节性动态的控制机理尚不明确.本研究在天鹅洲湿地采集2个水文地质钻孔的35件沉积物样品、12个分层监测井不同季节的共72组地下水样和18组地表水样，通过水位-水化学监测、沉积物地球化学组成分析和砷、铁形态表征探究天鹅洲湿地地下水中砷的时空分布规律及控制机理.研究发现天鹅洲湿地地下水砷含量为1.08~147 μg/L，牛轭湖外侧浅井（10 m）地下水砷含量普遍高于深井（25 m）和牛轭湖内侧浅井（10 m）、深井（25 m）地下水，枯水期和平水期的砷含量高于丰水期.牛轭湖外侧浅层地下水系统具有更厚的粘土、亚粘土沉积，沉积物中总砷、强吸附态砷和易还原的铁氧化物的含量更多，吸附砷的水铁矿等无定形铁氧化物还原性溶解导致砷释放进入地下水中.枯水期天鹅洲湿地底部向牛轭湖外侧浅层含水层输送不稳定的有机质，使天鹅洲湿地地下水-地表水界面成为砷释放的热点区域.丰水期时牛轭湖外侧含水层受长江补给的影响，还原环境发生改变使地下水中的砷和铁被氧化固定从而不利于砷向地下水释放.Abstract: High arsenic groundwater not only directly endangers water supply safety, but also affects the water quality of wetlands and thus threatens the ecological safety of wetlands through the long-term interactions between groundwater and surface water. The spatial distribution of arsenic in groundwater in the Tian-E-Zhou wetland in the middle reach of the Yangtze River has been reported to be wide, but the spatial distribution characteristics of arsenic in groundwater in the Tian-E-Zhou wetland in the middle reach of the Yangtze River are still not clear, and the control mechanism of the interaction between the wetland and groundwater on the seasonal dynamics of arsenic in groundwater is not clear. In this study, 35 sediment samples from 2 hydrogeological boreholes, a total of 72 sets of groundwater samples and 18 sets of surface water samples from 12 stratified monitoring wells in different seasons were collected in the Tian-E-Zhou wetland, and the spatial-temporal distribution patterns and control mechanisms of arsenic in groundwater in the Tian-E-Zhou wetland were investigated by water level-water chemistry monitoring, sediment geochemical composition analysis and arsenic-iron morphological characterization. It was found that the arsenic content of groundwater in the Tian-E-Zhou wetland ranged from 1.08 to 147.00 μg/L. The arsenic content of groundwater in shallow wells (10 m) under the outer side of the Oxbow Lake was generally higher than that in deep wells (25 m) and groundwater under the inner side of Oxbow Lake, and the arsenic content in the non-monsoon was higher than that in the monsoon. The shallow groundwater system under the outer side of the Oxbow Lake has thicker clayey and sub-clayey deposits with higher total arsenic, strongly adsorbed state arsenic and easily reduced iron oxides in the sediments, and reductive dissolution of amorphous iron oxides such as ferrihydrite minerals that adsorb arsenic leads to the release of arsenic into the groundwater. The transport of reactive organic matters from the bottom of the Tian-E-Zhou wetland to the shallow aquifer outside the Oxbow Lake during the non-monsoon makes the groundwater-surface water interface of the Tian-E-Zhou wetland a hot spot area for arsenic release. During the monsoon, the aquifer on the outer side of the Oxbow Lake is influenced by the recharge of the Yangtze River, and the reduction environment is changed so that the arsenic and iron in the groundwater are fixed by oxidation, which is detrimental to the release of arsenic to the groundwater.
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图 1 天鹅洲湿地监测井地理位置和典型水文地质剖面图
Fig. 1. Locations of monitor wells and hydrogeological sections in the Tian-E-Zhou wetland
图 2 天鹅洲湿地地下水、地表水Piper三线图（a）及Cl/Br图示（b）
Cl/Br图示中的红色小正方形代表污水端元，其数据来源于美国的一处化粪池的渗滤液Panno et al.（2006），海水混合线、稀释补给端元等参照McArthur et al.（2012）
Fig. 2. Piper diagram (a) of groundwater and surface water and Cl/Br diagram (b) of the Tian-E-Zhou wetland
图 3 天鹅洲湿地地下水砷的时空分布特征
a.砷的空间分布特征；b.牛轭湖外侧砷的时间变化特征；c.牛轭湖内侧砷的时间变化特征
Fig. 3. Spatial and temporal distribution of As in groundwater in the Tian-E-Zhou wetland
图 4 天鹅洲湿地典型钻孔（C3、C5）沉积物砷、铁形态含量百分比图
Fig. 4. Occurrence forms of As and Fe in typical borehole (C3、C5) sediments of the Tian-E-Zhou wetland
图 5 天鹅洲湿地地下水As含量与Fe2+（a）、DOC（b）、Cl/Br（c）的关系
Fig. 5. The relationship between As in groundwater and Fe2+ (a), DOC (b), Cl/Br (c) of the Tian-E-Zhou wetland
图 6 天鹅洲湿地高砷区和低砷区典型钻孔(C3、C5)岩性及对应沉积物地化指标分布图
Fig. 6. Distribution of lithology and geochemical indicators of sediments in typical boreholes (C3、C5) in both high and low arsenic areas of the Tian-E-Zhou wetland
图 7 天鹅洲湿地地下水与天鹅洲、长江（地表水‒地下水）水位差值（a）和天鹅洲地下水Eh随时间变化图（b）
Fig. 7. Difference in surface water and groundwater level (SW-GW) between Yangtze River and the Tian-E-Zhou wetland(a) and groundwater Eh variation in the Tian-E-Zhou wetland(b)
图 8 天鹅洲湿地地下水系统砷季节性变化控制机理概念模型
a. 枯水期（2020年12月~ 2021年2月）；b. 丰水期（2021年4月~ 2021年8月）
Fig. 8. Conceptual model of the control mechanism of arsenic seasonal variation in the groundwater system of the Tian-E-Zhou wetland
表 1 天鹅洲水样水化学统计表
Table 1. Statistics of hydrochemistry of the Tian-E-Zhou water samples
指标 牛轭湖外侧浅井（10 m） 牛轭湖外侧深井（25 m） 牛轭湖内侧浅井（10 m） 牛轭湖内侧深井（25 m） 天鹅洲湿地（牛轭湖） 长江 最大值 最小值 中位数 最大值 最小值 中位数 最大值 最小值 中位数 最大值 最小值 中位数 最大值 最小值 中位数 最大值 最小值 中位数 pH 7.46 6.92 7.12 7.54 6.93 7.12 7.68 6.73 7.40 7.58 6.72 7.20 8.62 7.76 8.15 8.31 7.79 8.05 Eh（mV） ‒3.50 ‒103 ‒88.0 31.0 ‒91.3 ‒66.0 ‒46.7 ‒133 ‒89.5 ‒3.50 ‒101 ‒56.0 89.8 38.7 66.2 106 3.00 43.05 EC（µs/cm） 1 275 606 856 1 149 840 974.5 827 413 737 897 648 785 464 325 384 413 322 371 TDS（mg/L） 897 402 540 782 577 654 541 261 478 675 396 523 334 218 255 265 188 237 DOC（mg/L） 19.4 6.78 13.2 12.4 4.31 8.58 25.6 4.16 6.62 9.23 3.19 6.00 14.3 4.35 5.71 4.08 0.81 3.19 NH4-N（mg/L） 11.9 0.37 9.35 1.35 0.75 0.89 8.60 1.85 3.43 3.10 0.57 0.74 0.41 0.09 0.19 0.96 0.05 0.22 K（mg/L） 5.95 2.90 4.74 4.19 2.86 3.7 9.56 3.27 4.71 3.5 2.66 3.13 6.62 4.30 5.87 3.02 2.42 2.76 Na（mg/L） 57.6 15.7 33.4 52.6 11.8 24.2 57.4 5.77 24.6 41.8 6.29 18.8 56.7 6.68 15.3 33.6 11.2 22.5 Ca（mg/L） 173 87.3 116 217 149 178 141 51.2 113 170 105 130 68.0 38.5 49.2 52.6 47.6 48.6 Mg（mg/L） 63.8 25.8 40.2 52.1 34.8 43.1 39.9 10.2 32.3 41.9 29.2 34.1 20.7 13.8 15.89 12.11 10.31 11.91 HCO3-（mg/L） 896 340 583 868 700 766 553 298 514 649 459 561 237 155 206 159 136 148 SO42-（mg/L） 71.5 ND 27.3 38.3 ND 13.7 54.7 ND 25.4 118 0.78 38.0 93.6 17.9 37.2 81.0 17.9 49.0 NO3 -（mg/L） 0.18 ND ND ND ND ND 0.05 ND ND 0.73 ND ND 6.29 ND 0.32 11.8 0.54 7.16 Cl -（mg/L） 59.6 5.51 16.3 8.83 0.70 3.02 68.9 14.2 24.4 48. 6 1.24 5.62 33.8 6.15 16.0 29.9 12.3 18.9 Br（mg/L） 1.53 0.14 0.27 1.19 0.13 0.17 0.06 0.02 0.05 0.05 0.02 0.04 0.05 0.02 0.04 0.05 0.01 0.02 Cl/Br 353 3.95 94.5 39.2 3.73 6.76 1 327 315 669 976 24.4 259 977 152 563 3 066 348 1 217 P（µg/L） 578 18.9 97.3 239 23 131 590 ND 69.4 368 3.96 102 117 33.13 43.7 286 62.5 114 As（µg/L） 147 10.1 67.8 54.6 4.62 11.6 59.6 16.2 22.7 26.3 1.08 13.8 4.68 2.35 3.25 1.92 1.49 1.83 Fe（mg/L） 12.8 1.36 7.75 4.81 0.36 2.05 4.34 0.01 2.48 2.12 0.03 0.64 0.13 0.01 0.03 0.05 0.01 0.02 Fe2+（mg/L） 11.3 1.00 7.38 4.55 0.27 2.02 4.30 0.01 2.72 1.89 ND 0.71 ‒ ‒ ‒ ‒ ‒ ‒ S2-（mg/L） 307 ND 38.5 46.0 ND 5.00 276 ND 33.5 323 ND 6.00 ‒ ‒ ‒ ‒ ‒ ‒ 注：“ND”表示低于检测限，“‒”代表数据未获取. 
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