Fluorine enrichment pattern of groundwater in the lower reaches of the Yellow River in southwestern Shandong Province and influencing factors
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摘要:
鲁西南平原位于黄河下游，现阶段对该区地下水水化学成因及其对地下水中F元素富集影响机理的研究较少。该研究以鲁西南平原沿黄河地带地下水为主要研究对象，采集浅层地下水样品36件，深层地下水样品16件，黄河水样品2件进行全分析测试；通过统计、相关性分析、水化学模拟等方法手段，计算氯碱指数（CAI），绘制Durov图、Gibbs图、Ca2+/Na+–Mg2+/Na+图、log10(Ca2+)activity–log10(F−)activity图等图件，分析了研究区地下水水化学成因及其富氟机理。结果显示，鲁西南沿黄区浅层及深层地下水化学类型均以HCO3−Na为主，整体偏碱性，地下水氟含量分别为1.59 mg/L、2.35 mg/L，深层水氟含量水平变化程度低于浅层；区内浅层地下水氟与Ca2+含量呈显著负相关，与pH值呈显著正相关，深层地下水中氟与Na+、TDS值呈显著正相关。鲁西南沿黄区地下水氟含量主要来源于萤石（CaF2）的溶解，受水岩作用和阳离子交换作用共同控制下的Ca2+含量制约。此研究揭示了黄河下游主要地下水含水层中氟富集规律和影响因素。
Abstract:The southwestern plain of Shandong Province is located in the lower reaches of the Yellow River, and there are few studies on the chemical genesis of groundwater in this region and the mechanism of its influence on fluorine enrichment in groundwater at this stage. In this study, 36 shallow groundwater samples, 16 deep groundwater samples and 2 Yellow River water samples were collected for comprehensive analysis and testing. By means of statistical, correlation analysis and water chemistry simulation, the chlor−alkali index (CAI) , Durov diagram, Gibbs diagram, Ca2+/Na+−Mg2+/Na+ diagram, log10(Ca2+)activity−log10(F−) activity diagram were constructed, and then the causes of groundwater chemistry and its fluoride enrichment mechanism in the study area were analyzed. The results showed that the chemical types of both shallow and deep groundwater in the study area were mainly HCO3−Na, indicating the overall alkaline, the fluorine content of groundwater was 1.59 mg/L and 2.35 mg/L, respectively, and the level of fluorine content in deep water varied less than that in shallow water. The fluorine content in shallow groundwater in the area was significantly negatively correlated with Ca2+ content and positively correlated with pH value. The fluorine content in deep groundwater was significantly and positively correlated with Na+ and TDS values. The chemical composition of groundwater in the study area is mainly controlled by water−rock action and cation exchange, and the fluorine content of groundwater mainly comes from the dissolution of fluorite (CaF2), and is controlled by Ca2+ content. This study revealed the fluorine enrichment laws and influencing factors in the main groundwater aquifers in the lower reaches of the Yellow River.
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表 1 研究区主要水体化学组分统计
Table 1. Statistics of chemical components of main water bodies in the study area
ρB/
(mg·L−1)黄河水 浅层地下水（n=36） 深层地下水（n=16） 上游 下游 最大值 最小值 平均值 变异系数 最大值 最小值 平均值 变异系数 K+ 3.68 4.21 2.75 0.04 0.74 0.77 1.88 0.41 0.66 0.51 Na+ 96.74 91.37 1853.12 68.44 391.64 1.03 350.53 184.83 274.29 0.14 Ca2+ 59.59 55.18 361.57 8.45 86.39 0.95 28.31 3.47 8.27 0.68 Mg2+ 29.16 28.09 766.19 12.40 115.71 1.24 18.52 1.96 9.53 0.55 Cl− 89.55 93.49 2542.55 21.26 381.45 1.51 150.74 32.14 92.52 0.38 SO42− 160.54 150.21 4085.37 11.67 420.59 1.90 206.97 59.57 125.21 0.39 HCO3− 224.62 195.00 1404.46 419.61 695.03 0.30 530.69 375.18 449.35 0.10 CO32− 0.00 0.00 0.00 0.00 0.00 - 55.84 0.00 14.28 1.38 F− 0.23 0.32 4.52 0.19 1.59 0.64 3.52 1.08 2.35 0.28 CO2 0.00 0.00 15.21 0.00 6.99 0.50 0.00 0.00 0.00 - TDS 573.38 538.13 9986.68 520.96 1767.28 1.11 1018.90 627.64 768.59 0.15 pH 8.31 8.32 8.33 6.97 7.62 0.04 8.69 8.17 8.36 0.02 
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表 2 研究区地下水氟含量与主要化学指标相关性
Table 2. Correlation between fluoride content and main chemical indexes of groundwater in the study area
水体 相关性参数 Na+ Ca2+ Mg2+ Cl− SO42− HCO3− pH H2SiO3 TDS 浅层地下水
n=36r −0.07 −0.60 −0.31 −0.30 −0.22 0.30 0.55 −0.17 −0.23 p 0.70 0.00 0.07 0.08 0.21 0.08 0.00 0.32 0.19 深层地下水
n=16r 0.69 −0.34 0.22 0.45 0.41 0.27 0.13 0.15 0.61 p 0.00 0.19 0.40 0.08 0.12 0.31 0.63 0.57 0.01 注： r值带符号“−”，代表负相关关系，否则为正相关关系。相关性统计学显著水平：p≥0.05，不显著；p＜0.05，显著；p＜0.01，非常显著
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表 3 研究区各主要水体矿物饱和指数模拟结果（模拟温度20℃）
Table 3. Statistics of simulation results of mineral saturation index of main water bodies in the study area
水体 SI方解石 SI白云石 SI石膏 SI萤石 黄河水 上游 0.85 1.64 −1.54 −2.37 下游 0.78 1.51 −1.59 −2.10 浅层地下水
（n=36）最大值 0.90 2.29 −0.19 −0.29 最小值 0.18 0.58 −2.81 −2.26 平均值 0.53 1.38 −1.70 −1.13 变异系数 0.38 0.29 −0.35 −0.49 深层地下水
（n=16）最大值 0.86 1.73 −2.00 −1.03 最小值 0.11 0.28 −3.03 −1.93 平均值 0.28 0.90 −2.61 −1.35 变异系数 0.59 0.39 −0.11 −0.20 注： SI为矿物饱和指数
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