Characterization and causes of interannual variation of antimony contamination in groundwater of a typical antimony mining area
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摘要:
湘中锡矿山锑矿区重金属污染问题突出，近年来矿区大力实施废渣综合整治和生态修复工程，但地下水污染修复成效未知。通过2013—2022年连续10 a 采集的锡矿山锑矿区地下水样品，运用水化学分析、离子相关性分析、地统计学等方法，对地下水化学特征、锑污染年际变化特征、锑污染来源和途径进行了系统研究。结果显示：（1）锡矿山锑矿区地下水水化学类型主要为HCO3·SO4—Ca型，地下水水化学组分的形成过程受固废淋滤和盐岩溶解控制；（2）矿区泥盆系上统佘田桥组、锡矿山组以及矿区外围下石炭统3个灰岩裂隙含水层受到不同程度的锑污染，尤其是佘田桥组含水层，锑质量浓度均值达7.139 mg/L，受辉锑矿氧化影响显著，而锡矿山组、下石炭统含水层锑的来源主要受尾渣、废石等固体废弃物淋滤控制；（3）10 年间佘田桥组地下水锑质量浓度均值差异较大，2013—2015年，锑质量浓度均值为13.31 mg/L，逐年下降，2016—2018年锑质量浓度均值为7.28 mg/L，逐年略升，2019—2022年锑质量浓度均值为6.06 mg/L，整体呈下降趋势。分析表明矿区生态环境逐步转好，研究成果可为矿区生态修复工程实施成效评估、矿区重金属污染防治提供科学依据。
Abstract:Heavy metal pollution is a prominent problem in the antimony mining area of Xikuangshan in central Hunan. In recent years, integrated waste remediation and ecological restoration projects have been vigorously implemented in mining areas, but the effectiveness of groundwater pollution remediation is unknown. Groundwater samples collected from the antimony mining area for 10 consecutive years from 2013 to 2022 are used to systematically study the chemical characteristics of groundwater, the inter-annual variation characteristics of antimony pollution, and the sources and pathways of antimony contamination by the hydrochemistry analysis, ion correlation analysis, and geostatistics. The results show that (1) the HCO3·SO4—Ca type is the main hydrochemical type of groundwater in Xikuangshan, and the formation process of chemical components in the groundwater is controlled by solid waste leaching and salt rock dissolution. (2) Three aquifers in the mining area are contaminated with antimony to different degrees, especially the Shetianqiao Formation aquifer, with an average antimony concentration of 7.139 mg/L, which is significantly affected by the oxidation of pyroxene. The sources of antimony in the Xikuangshan Formation and the Lower Carbonifer aquifer are mainly controlled by the leaching of solid waste such as tailings and waste rocks. (3) The average value of antimony mass concentration in groundwater in the Shetianqiao Formation aquifer varies greatly during the 10 years. From 2013 to 2015, the average value of antimony concentration was 13.31 mg/L, decreasing year by year. From 2016 to 2018, the average value of antimony concentration is 7.28 mg/L, increasing slightly year by year. From 2019 to 2022 the average value of antimony concentration is 6.06 mg/L, with an overall decreasing trend. Analysis shows that the ecological environment in the mining area is gradually improving. This study will provide a scientific basis for assessment of the effectiveness of the implementation of ecological restoration projects in mining areas, as well as the prevention and control of heavy metal pollution in mining areas.
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Key words:
- antimony mining area /
- groundwater /
- heavy metal /
- antimony contamination /
- ecological restoration
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表 1 样品测试指标及方法
Table 1. Sample testing index and methods
指标 仪器 方法 pH 多参数水质分析仪
（HACH-HQ40d）现场测定 K+、Na+、Ca2+、Mg2+、
Sb质量浓度电感耦合等离子体发射光
谱仪（ICAP 7000 Series）《水质 32元素的测定
电感耦合等离子体发射光谱法》(HJ 776—2015)[27]Cl−质量浓度 离子色谱仪（ICS-900） 《水质 无机阴离子（F −、Cl−、 ${\rm{NO}}_2^- $ 、Br−、${\rm{NO}}_3^-$ 、${\rm{PO}}_4^{3-} $ 、${\rm{SO}}_3^{2 -} $ 、${\rm{SO}}_4^{2 -} $ ）
的测定离子色谱法》(HJ 84—2016)[28]${\rm{HCO}}_3^- $ 质量浓度滴定管0.01~50.00 mL 《地下水质分析方法 第49部分：碳酸根、
重碳酸根和氢氧根离子的测定 滴定法》(DZ/T 0064.49—2021)[29]${\rm{SO}}_4^{2 -} $ 质量浓度可见分光光度计（721 G） 《地下水质分析方法 第64部分：
硫酸盐的测定乙二胺四乙酸二钠—钡滴定法》(DZ/T 0064.64—2021)[30]
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表 2 各年度地下水样品采集情况统计
Table 2. Statistics of groundwater samples collection from 2013 to 2022
编号 水点类型 所处含水层 2013年7月 2014年6月 2015年7月 2016年9月 2017年12月 2018年6月 2019年6月 2020年7月 2021年9月 2022年10月 小计/组 Ds1 泉 佘田桥组 √ √ √ √ √ √ √ √ √ √ 10 Ds2 泉 佘田桥组 √ √ √ √ √ 5 Ds3 泉 佘田桥组 √ √ √ √ √ 5 Ds4 泉 佘田桥组 √ √ √ √ √ √ √ √ √ 9 Ds5 泉 佘田桥组 √ √ √ √ √ √ 6 Ds6 泉 佘田桥组 √ √ √ √ √ 5 Ds7 钻井 佘田桥组 √ √ √ √ √ √ 6 Ds8 钻井 佘田桥组 √ √ √ √ √ √ 6 Ds9 钻井 佘田桥组 √ √ √ √ 4 Ds10 钻井 佘田桥组 √ √ √ √ √ √ √ 7 Ds11 钻井 佘田桥组 √ √ √ √ 4 Dx1 泉 锡矿山组 √ √ √ √ √ √ √ √ √ √ 10 Dx2 泉 锡矿山组 √ √ √ √ √ √ √ √ √ √ 10 Dx3 泉 锡矿山组 √ √ √ √ √ √ √ 7 Dx4 泉 锡矿山组 √ √ √ √ √ √ √ √ √ 9 Dx5 泉 锡矿山组 √ √ √ √ √ √ √ √ 8 Dx6 泉 锡矿山组 √ √ √ √ √ √ √ √ √ √ 10 Dx7 泉 锡矿山组 √ √ √ √ √ √ 6 Dx8 泉 锡矿山组 √ √ √ √ √ √ √ √ √ 9 Dx9 钻井 锡矿山组 √ √ √ √ √ √ √ 7 Dx10 钻井 锡矿山组 √ √ √ √ √ √ √ 7 Dx11 钻井 锡矿山组 √ √ √ √ 4 Dx12 钻井 锡矿山组 √ √ √ √ √ 5 Dx13 钻井 锡矿山组 √ √ √ √ √ 5 Dx14 钻井 锡矿山组 √ 1 Dx15 钻井 锡矿山组 √ √ √ √ √ 5 C1 泉 下石炭统 √ √ √ √ √ √ √ √ 8 C2 泉 下石炭统 √ √ √ √ 4 C3 钻井 下石炭统 √ √ √ √ √ √ √ 7 C4 泉 下石炭统 √ √ 2 合计/组 12 15 16 22 26 18 16 25 21 20 191
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表 3 研究区地下水化学指标统计
Table 3. Statistics of groundwater chemistry in the study area
年份 样品
数量/组层位 物化参数 pH 质量浓度/（mg·L−1） TDS/（mg·L−1） K+ Na+ Ca2+ Mg2+ Cl− ${\rm{SO}}_4^{2 -} $ ${\rm{HCO}}_3^- $ 2013年 12 佘田桥组 均值 7.83 4.29 8.79 79.27 5.05 12.16 118.06 121.28 426.17 锡矿山组 均值 8.01 0.94 5.49 94.36 9.37 7.41 131.25 180.39 445.32 下石炭统 均值 8.20 0.60 1.98 96.71 4.71 5.70 81.94 202.13 415.52 2014年 15 佘田桥组 均值 6.83 2.33 22.88 50.48 3.95 4.69 125.49 72.00 313.20 锡矿山组 均值 7.21 0.90 17.13 71.38 7.66 2.74 144.08 117.84 378.67 下石炭统 均值 7.27 0.53 12.47 63.49 2.91 1.18 97.17 123.57 318.28 2015年 16 佘田桥组 均值 8.42 3.15 19.37 51.23 5.76 5.69 77.95 126.98 259.45 锡矿山组 均值 8.01 1.57 13.48 75.00 6.50 3.96 72.77 196.00 291.75 下石炭统 均值 7.55 0.61 2.71 88.15 3.44 0.94 65.40 205.00 276.31 2016年 22 佘田桥组 均值 7.34 3.95 41.48 72.63 8.66 21.44 148.99 137.97 380.53 锡矿山组 均值 7.67 2.37 14.70 94.23 9.44 5.24 135.12 204.92 378.55 下石炭统 均值 7.41 1.20 6.93 100.13 12.35 1.21 87.40 267.67 349.09 2017年 26 佘田桥组 均值 7.37 — — — — 8.08 126.90 — 243.11 锡矿山组 均值 7.74 — — — — 4.58 134.92 — 273.80 下石炭统 均值 7.64 — — — — 13.09 252.07 — 355.33 2018年 18 佘田桥组 均值 6.84 — — — — 4.91 248.83 — 530.67 锡矿山组 均值 7.30 — — — — 4.74 207.62 — 560.73 下石炭统 均值 7.24 — — — — 1.40 55.50 — 298.00 2019年 16 佘田桥组 均值 6.73 — — — — 4.74 198.66 — 422.80 锡矿山组 均值 7.47 — — — — 5.37 113.47 — 402.40 下石炭统 均值 7.42 — — — — 0.46 23.10 — 192.00 2020年 25 佘田桥组 均值 7.38 5.63 25.97 113.62 9.70 9.18 206.29 187.12 506.51 锡矿山组 均值 7.27 2.03 8.89 119.61 10.80 4.29 133.48 233.14 417.57 下石炭统 均值 7.53 1.01 1.22 78.00 4.59 0.49 73.00 199.50 269.49 2021年 21 佘田桥组 均值 6.97 4.95 37.27 77.74 9.11 4.32 188.08 168.21 435.00 锡矿山组 均值 7.32 2.37 7.30 71.37 9.76 3.41 103.78 213.60 319.30 下石炭统 均值 7.33 0.75 1.83 61.53 7.69 0.41 62.00 245.67 266.67 2022年 20 佘田桥组 均值 7.89 3.30 38.42 106.22 13.54 7.55 193.08 176.62 487.83 锡矿山组 均值 8.00 1.49 7.86 119.10 11.68 4.69 116.45 218.91 375.82 下石炭统 均值 7.95 1.04 2.20 94.30 9.09 0.66 65.03 204.00 276.67 2013—
2022年191 佘田桥组 最小值 4.05 0.47 0.88 21.38 1.61 0.00 57.90 6.10 102.00 最大值 8.90 10.80 192.00 209.00 35.10 141.00 638.00 356.00 1110.00 均 值 7.31 4.14 28.66 81.75 8.64 6.94 173.64 154.78 397.88 标准差 0.85 2.65 36.73 41.18 6.51 8.36 130.85 102.98 207.80 锡矿山组 最小值 6.81 0.32 0.77 28.60 2.17 0.53 26.90 37.20 157.00 最大值 8.63 5.56 68.20 179.00 37.20 29.80 541.00 373.00 982.00 均 值 7.57 1.73 10.31 96.28 9.82 4.92 136.01 199.79 390.01 标准差 0.41 1.41 11.97 39.79 7.32 6.10 98.22 68.68 160.79 下石炭统 最小值 6.88 0.26 1.22 57.20 2.86 0.37 23.10 108.31 172.00 最大值 8.34 2.39 21.63 112.00 27.00 6.08 114.00 301.00 454.84 均 值 7.58 0.84 4.09 83.56 6.98 1.33 71.78 212.49 294.69 注：表中“—”为测试数据缺失。表中“标准差”为无量纲。下石炭统因为水样数据少（1~3个），不符合标准差使用条件，故未统计标准差。
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表 4 2013—2022年各含水层地下水Sb质量浓度统计
Table 4. Statistics of antimony concentrations in groundwater of each aquifer from 2013 to 2022
年份 佘田桥组 锡矿山组 下石炭统 数量
/个最小值
/（mg·L−1）最大值
/（mg·L−1）均值
/（mg·L−1）标准差 变异系数 数量
/个最小值
/（mg·L−1）最大值
/（mg·L−1）均值
/（mg·L−1）标准差 变异系数 数量
/个最小值
/（mg·L−1）最大值
/（mg·L−1）均值
/（mg·L−1）2013年 2 10.350 42.380 26.364 — — 8 0.020 0.986 0.258 0.307 1.192 2 0.032 0.097 0.064 2014年 5 1.205 39.160 9.755 16.468 1.688 8 0.012 2.775 0.504 0.929 1.844 2 0.012 0.222 0.117 2015年 6 0.890 13.100 3.813 4.649 1.219 8 0.001 0.360 0.119 0.138 1.165 2 0.004 0.520 0.262 2016年 9 0.048 46.100 6.730 14.830 2.204 10 0.006 0.540 0.165 0.173 1.045 3 0.017 0.130 0.089 2017年 11 0.051 44.700 7.011 13.144 1.875 13 0.007 0.470 0.165 0.170 1.032 2 0.009 0.018 0.014 2018年 6 0.067 34.000 8.105 12.951 1.598 11 0.001 3.080 0.524 0.896 1.711 1 0.460 0.460 0.460 2019年 5 0.040 18.500 6.476 7.585 1.171 10 0.015 16.500 1.930 5.139 2.662 1 0.270 0.270 0.270 2020年 9 0.086 20.800 6.036 7.299 1.209 14 0.008 1.040 0.359 0.409 1.065 2 0 0.117 0.059 2021年 8 0.470 24.100 5.284 8.005 1.515 10 0.004 0.850 0.244 0.238 0.977 3 0.017 0.037 0.025 2022年 6 0.019 28.800 6.445 11.068 1.717 11 0.003 0.920 0.202 0.271 1.341 3 0.008 0.011 0.009
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表 5 典型地下水采样点基本信息表
Table 5. Basic information of typical groundwater sampling points
编号 水点类型 含水岩组 位置 与污染源关系 水位标高/m Dx2 泉点 锡矿山组 北矿谭家社区 北矿宝大兴老矿山废石渣堆东侧 562 Dx4 泉点 锡矿山组 北矿七里江社区半山坡 — 593 Dx6 泉点 锡矿山组 南矿泉山村玄山河西侧 物华锑矿采矿废石堆南西450 m 358 Dx8 泉点 锡矿山组 南矿泉山村陈家湾 — 446 Ds4 泉点 佘田桥组 北矿新生村 北矿宝大兴老矿山露采区北侧坡脚 535 Ds8 水文钻井 佘田桥组 北矿老陶唐北 北矿宝大兴老矿山露采区东侧坡脚 538 Ds10 水文钻井 佘田桥组 南矿黄光村 南矿飞水岩露采区历史废渣堆下 430 Dx9 水文钻井 锡矿山组 北矿东十八茅湾 — 611 C3 水文钻井 下石炭统 北矿谭家社区/揭露F75 — 581
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