Isotopic Indication of Spatial Heterogeneity of Arsenic in Shallow Groundwater of Middle Yangtze River Lacustrine Plain
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摘要: 近年来陆续有报道发现长江中游河湖平原广泛分布着高砷地下水，鄱阳湖平原与江北平原（古彭蠡泽）作为长江中游南北两岸典型的河湖平原，其地下水资源丰富，但砷的空间分布规律尚不清楚，区域供水安全存在风险.本研究在两个区域系统采集98个浅层地下水（< 40 m）样品和8个地表水样品，通过水化学、氢氧稳定同位素分析，查明地下水中砷的空间分布异质性及其影响因素.研究发现江北平原浅层地下水砷含量为0.65~956.72 μg/L（平均值210.78 μg/L），高砷地下水集中分布于长江古河道；鄱阳湖平原浅层地下水砷含量为0.09~267.45 μg/L（平均值11.85 μg/L），高砷地下水仅分布于赣江三角洲局部地区.江北平原地下水δD与δ18O值相对鄱阳湖平原更偏负，且与地表水的差异更大.地下水化学及主成分分析结果表明物源和含水层结构差异是影响鄱阳湖平原和江北平原砷空间分布异质性的关键因素，来自长江物源的古彭蠡泽区域沉积物为高砷含水层的形成提供了物质来源，湖相含水层中含砷铁氧化物的还原性溶解是地下水砷富集的主要过程.地下水氢氧稳定同位素指示江北平原较鄱阳湖平原地下水赋存环境更封闭，地下水循环交替速度缓慢，有利于砷的富集.Abstract: In recent years, it has been reported that high arsenic groundwater is widely distributed in the the middle Yangtze River lacustrine plain. The Poyang Lake plain (PYP) and the Jiangbei plain (ancient Pengli Lake, JBP) are typical lacustrine plains rich in groundwater resources on the northern and southern sides of the middle reach of the Yangtze River. However, the spatial distribution of groundwater arsenic in these regions has not been clearly studied, which posed potential risks to regional water supply security. In this study, 98 shallow groundwater samples and 8 surface water samples were collected in these two regions. The spatial heterogeneity of arsenic in groundwater and its controlling factors were identified by hydrochemistry and stable isotope analysis. The arsenic contents of shallow groundwater in JBP range from 0.65 to 956.72 μg/L (average 210.78 μg/L), and the high arsenic groundwater is mainly distributed in the ancient Yangtze River channel. The arsenic contents of shallow groundwater in PYP range from 0.09 to 267.45 μg/L (average 11.85 μg/L), and the high arsenic groundwater is only distributed in parts of Ganjiang River delta. Stable water isotope composition (δD and δ18O) of groundwater samples from the JBP is more negative and significantly different from surface water relative to the PYP. Multivariate statistical results of groundwater chemistry data indicate that the differences of provenance and aquifer structure are the key factors affecting arsenic spatial heterogeneity in shallow groundwater in PYP and JBP, the microbially mediated reductive dissolution of arsenic-bearing iron minerals leads to arsenic release in groundwater. Groundwater arsenic in the Jiangbei plain is supposed to be originated from the sediments from ancient Pengli area of Yangtze River provenance. The stable isotopic signatures of hydrogen and oxygen in groundwater indicate that the aquifer environment in JBP is closer and the groundwater circulation and alternation speed is slower compared with the PYP, which is more conducive to arsenic release and enrichment in the groundwater.
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Key words:
- groundwater /
- arsenic /
- hydrogen and oxygen stable isotopes /
- Poyang Lake plain /
- ancient Pengli Lake /
- geochemistry
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图 1 研究区采样点分布及水文地质剖面
Fig. 1. Locations of sampling sites and hydrogeological sections in the study area
图 2 研究区地表水-地下水Piper三线图
Fig. 2. Piper diagram of groundwater and surface water samples of both PYP and JBP
图 3 研究区地表水-地下水稳定氢氧同位素关系
1.当地大气降雨线；2.江北平原地下水拟合线；3.鄱阳湖平原地下水拟合线；4.江北平原；5.鄱阳湖平原；6.长江；7.地下水；8.河流；9.湖水
Fig. 3. The relationships between stable hydrogen and oxygen isotopes in groundwater and surface water samples of both PYP and JBP
图 4 研究区地下水中砷的浓度分布
Fig. 4. Distribution of As concentration in water samples of both PYP and JBP
图 5 研究区地下水主成分荷载
Fig. 5. Principal component load of groundwater samples of both PYP and JBP
图 6 研究区地下水中As与DOC、菱铁矿饱和指数的关系
Fig. 6. The plots of As concentrations and DOC concentrations and siderite saturation index in groundwater
图 7 研究区地下水18O同位素区域分布
Fig. 7. The distribution of groundwater 18O values both in PYP and JBP
图 8 研究区地下水δ18O与TDS关系
Fig. 8. Relationship between total dissolved solids and δ18O of water samples
图 9 研究区地下水18O与Cl/Br关系
Fig. 9. Relationship between δ18O and Cl/Br of groundwater in study area
表 1 鄱阳湖平原及江北平原地下水水化学特征
Table 1. Water chemistry of groundwater from Poyang Lake plain and Jiangbei plain
指标 鄱阳湖平原 江北平原 最小值 最大值 平均值 标准差 标准差 变异系数 最小值 最大值 平均值 标准差 变异系数 pH 4.70 7.42 6.06 0.61 0.61 0.10 6.66 7.26 6.97 0.14 0.02 EC (μS/cm) 55.50 612.00 246.69 135.68 135.68 0.55 292.00 1 148.00 751.45 180.35 0.24 Eh (mV) -137.00 322.50 152.39 121.91 121.91 0.80 -174.80 181.20 -50.31 114.71 -2.28 Fe2+(mg/L) ND 27.00 2.89 6.59 6.59 2.28 ND 14.75 5.03 4.02 0.80 NH4-N(mg/L) ND 23.00 1.09 3.29 3.29 3.02 0.01 15.60 3.37 3.13 0.93 DOC(mg/L) ND 4.54 1.53 1.07 1.07 0.70 1.98 16.83 6.57 2.69 0.41 Ca (mg/L) 2.19 105.79 23.80 19.75 19.75 0.83 38.49 209.91 137.91 40.00 0.29 Na (mg/L) 3.08 47.67 13.45 9.68 9.68 0.72 7.28 84.09 19.81 13.27 0.67 Mg (mg/L) 0.95 19.50 6.13 3.98 3.98 0.65 14.24 50.50 32.91 9.21 0.28 Cl- (mg/L) 0.52 147.37 20.28 23.52 23.52 1.16 0.92 72.74 12.59 15.86 1.26 NO3- (mg/L) 0.01 111.71 19.92 27.09 27.09 1.36 0.01 94.64 9.84 21.94 2.23 SO42- (mg/L) 0.01 47.71 10.96 13.70 13.70 1.25 0.01 79.34 11.49 21.72 1.89 HCO3- (mg/L) 9.19 290.91 95.57 69.77 69.77 0.73 17.24 862.01 565.30 203.51 0.36 As (µg/L) 0.09 267.45 11.85 38.63 38.63 3.26 0.65 956.72 210.78 227.64 1.08 Fe (mg/L) 0.01 48.08 5.82 12.98 12.98 2.23 0.01 20.30 6.63 5.57 0.84 Mn (mg/L) 0.01 21.21 1.34 3.08 3.08 2.30 0.01 3.48 0.47 0.61 1.30 注：ND.表示低于检出限. 
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表 2 鄱阳湖平原及江北平原地下水因子贡献率
Table 2. Contribution ratios of groundwater factors from PYP and JBP
指标 江北平原 鄱阳湖平原 主因子方差 PC1 PC2 PC3 主因子方差 PC1 PC2 PC3 Ca 0.890 0.613 0.687 -0.204 0.827 0.817 -0.147 -0.372 Mg 0.871 0.508 0.776 0.100 0.613 0.690 -0.188 -0.318 Na 0.770 -0.431 0.712 0.277 0.816 0.580 -0.609 0.331 HCO3- 0.772 -0.651 0.444 0.388 0.841 0.647 -0.174 0.626 Cl- 0.917 0.700 0.593 -0.277 0.886 0.779 0.299 -0.436 SO42- 0.628 -0.780 0.102 0.097 0.828 0.266 -0.655 0.573 NO3- 0.821 -0.869 0.220 0.130 0.700 0.541 -0.512 -0.382 As 0.578 0.639 -0.243 0.333 0.766 0.494 0.692 0.207 Fe 0.741 0.717 -0.305 0.365 0.774 0.426 0.705 0.310 NH4-N 0.709 0.576 0.018 0.613 0.707 0.416 0.701 0.206 贡献率(%) 43.529 23.414 10.021 34.692 27.060 15.846 累计贡献率(%) 43.529 66.943 76.964 34.692 61.752 77.598
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