Mobilization Mechanisms of High Fluorine and Iodine Groundwater in the Northwest Shandong Plain
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摘要:
地下水作为鲁西北平原的主要水源，查明高氟、高碘地下水的成因和联系十分必要，可为当地的饮用水安全及解决地方病的研究提供借鉴。目前中国对鲁西北地区浅层高氟地下水的研究较多，但对深层高氟地下水的成因、高氟地下水和高碘地下水的联系有待加强。本文旨在揭示鲁西北平原地下水中氟与碘的空间分布特征，推测高氟地下水的形成机制，查清碘在地下水系统中富集的关键水文地球化学过程，探讨地下水中高氟与高碘的关系。采集浅层（0～55m）、中层（55～225m）、深层（＞225m）地下水样品326件，并对18个水化学参数进行层次聚类分析，将地下水样品划分为高氟地下水、高碘地下水和高氟高碘地下水。再结合常规水化学指标和沉积物组分特征进行相关性分析，探讨高氟、高碘地下水的成因及联系。结果表明：高氟地下水与高碘地下水通常伴生出现，且高氟地下水和高碘地下水分布区水化学环境类似，高氟地下水主要集中在地面以下0～40m、50～110m以及225～305m深度内，其最大值（13.71mg/L）出现在地面以下110m深度处；高碘地下水主要集中在地面以下0～10m、55～65m以及225～285m深度内，其最大值（4.601mg/L）出现在234m深度处。含氟矿物萤石（CaF2）的溶解、强烈的蒸发浓缩作用、离子交换可能是高氟地下水的主要形成机制；地下水中的碘主要来自鲁西北平原沉积物中海洋生物和有机质，地下水受强烈的蒸发作用，水走盐留，水中碘浓度不断增加，沉积物淋溶以及氨氮和硫化物的还原溶解可能是导致地下水高碘的主要过程，弱碱性的水环境、还原条件和有机质的存在都是高碘水形成的重要因素。研究区强烈的蒸发浓缩作用、弱碱性的还原条件同时促进了氟和碘的富集。
Abstract:BACKGROUND Groundwater is the main water source in the Northwest Shandong Plain Province. It is necessary to find out the causes and connections of high fluorine and high iodine groundwater, which can provide reference for local drinking water safety and solving endemic diseases. At present, there is a lot of research on shallow high fluorine ground water in northwest Shandong, but little research focuses on the cause of deep high fluorine ground water, and the relationship between high fluorine groundwater and high iodine groundwater.
OBJECTIVES (1) To reveal the spatial distribution characteristics of fluorine and iodine in groundwater in the Northwest Shandong Plain; (2) To speculate the formation mechanism of high fluorine groundwater; (3) To identify the key hydrogeochemical processes of iodine enrichment in the groundwater system; (4) To explore the relationship between high fluorine and high iodine in groundwater.
METHODS Sediment samples were collected to investigate the lithology, mineral composition and elementary composition of the Northwest Shandong Plain. A total of 326 shallow (0-55m), middle (55-225m) and deep (>225m) groundwater samples were also collected. Hierarchical clustering analysis was applied to classify groundwater based on 18 water chemical parameters (pH, dissolved total solids, sulfate, chlorine, iron, volatile phenols, iodine, fluorine, arsenic, lead, calcium, magnesium, potassium, bicarbonate). The correlation analysis of water chemical parameters and sediment compositions was executed to investigate the causes of high fluorine and iodine groundwater. Furthermore, the calculation of the saturation index of fluorite further helped to determine the main formation mechanism of high fluorine groundwater. The water chemistry type of groundwater was obtained by drawing the piper three-line diagram, and combined with pH and other indicators, the main mechanism of the enrichment of deep high fluorine groundwater was studied. The piper three-line diagram and TDS relationship diagram were drawn to confirm the evaporation concentration mechanism of shallow high iodine groundwater. In addition, the hydrogeological conditions of the study area were analyzed, and the strong reducing environment of deep groundwater in the study area was judged by combining redox environmental sensitive factors, and the main reason for iodine enrichment in deep groundwater was obtained.
RESULTS The groundwater samples are divided into high fluorine groundwater, high iodine groundwater, and high fluorine and high iodine groundwater by hierarchical clustering analysis. High fluorine groundwater and high iodine groundwater have great similarities, and they are primarily the largest cluster. The high fluorine groundwater is mainly distributed at a depth of 0-40m, 50-110m and 225-305m below the ground surface, with the maximum value (13.7mg/L) occurring at a depth of 110m underground. The high iodine groundwater enriches at 0-10m, 55-65m and 225-285m deep, with the maximum value (4.6mg/L) appearing at 234m underground. Fluorine and iodine in groundwater are often associated, i.e., high fluorine groundwater also has higher iodine content. This is because the enrichment environmental conditions conducive to the two are similar. Strong evaporation concentration and leaching are the main processes leading to high fluorine and high iodine groundwater in the Northwest Shandong Plain. The fluorine-containing minerals and iodine-containing sediments in the shallow groundwater were continuously dissolved, which increased the content of fluorine and iodine in the groundwater. When rainfall occurs, fluorine and iodine in the soil dissolve or leach into the groundwater, resulting in its enrichment. In addition, the alkaline groundwater environment and high HCO3 − content can promote the dissolution of fluorine-containing minerals and the enrichment of iodine. The strong reducing groundwater environment and slow flow rate of deep groundwater can be conducive to fluorine enrichment. High fluorine groundwater and high iodine groundwater have similar chemical types, with the main anions of HCO3 and Cl, and the main cation of Na. In a weakly alkaline environment (pH=7-10), high fluorine and high iodine groundwater is formed through leaching and ion exchange.
CONCLUSIONS The dissolution of fluorine-rich minerals such as fluorite (CaF2), evaporation and ion exchange might be the dominant processes controlling fluorine mobilization in groundwater. The iodine in groundwater mainly comes from marine organisms and organic matter in sediments in the Northwest Shandong Plain. Evaporation, leaching and the reduction dissolution of ammonia nitrogen and sulfide are likely the primary processes leading to iodine enrichment. The weakly alkaline and reducing groundwater environment and the presence of organic matter are all important factors in the formation of high iodine groundwater. Generally, high fluorine groundwater also has high iodine content due to the similar formation mechanisms.
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图 2 浅层地下水样本的树状图。聚类分析时使用平均连接（组间），红色与绿色虚线为同型种线，对应Y分别为7.5和1.5。浅层地下水可分为高TDS区和低TDS区，具有高氟高碘特征的簇数目最多，其中S2、S3、S4、S6、S8、S13、S17、S18为低TDS组中的高氟高碘簇
Figure 2.
图 3 S1聚类树状图（红色虚线为同型种线，对应Y为5.5），浅层地下水最大聚类S1聚类结果显示S1-2、S1-3、S1-8、S1-10和S1-12为高氟高碘簇
Figure 3.
图 4 M1聚类树状图（红色与绿色虚线为同型种线，对应Y分别为5.5和1.5），中层地下水最大聚类M1中高氟高碘簇数目最多（M1-2、M1-3、M1-4、M1-5、M1-6、M1-7、M1-8、M1-9、M1-10、M1-12、M1-14、M1-15、M1-16、M1-17）
Figure 4.
图 5 深层地下水样本树状图（红色与绿色虚线为同型种线，对应Y分别为5.5和1.5），深层地下水高氟高碘簇数目最多（D1、D2、D4、D5、D6、D7、D10），最大氟浓度5.3mg/L（D7），最大碘浓度4.6mg/L（D1）
Figure 5.
图 7 高氟、高碘地下水piper三线图，浅层、中层、深层高氟地下水的水化学类型分别为HCO3·SO4·Cl-Na·Mg 型、SO4·Cl-Na·Mg型和HCO3-Na型，高碘地下水中主要阳离子为Na+和Ca2+，主要阴离子为Cl−和HCO3 −
Figure 7.
表 1 样品分析指标的测定方法、仪器、检出限和精密度
Table 1. Measurement method, instrument, detection limit and precision of analysis indicators for samples.
分析指标 测定方法和仪器 方法检出限 方法精密度（RSD） pH 现场测定（雷磁DZB-712型，上海仪电科学仪器股份有限公司） 0.01 1.0% HS−、NH4 +-N 现场测定（DR2010型，美国HACA公司） 0.0001mg/L 1.0% 钠 电感耦合等离子体发射光谱法
（Optima 8300型，美国PerkinElmer公司）0.001mg/L 0.5% 铁、锰、铜、锌、铝、铅 电感耦合等离子体发射光谱法
（Optima 8300型，美国PerkinElmer公司）0.00001mg/L 0.5% 砷、镉 电感耦合等离子体质谱法
（NexION 300X型，美国PerkinElmer公司）0.00001mg/L 1.0% 碘化物 电感耦合等离子体质谱法
（NexION 300X型，美国PerkinElmer公司）0.001mg/L 1.0% 氟化物、氨氮 离子色谱法（ICS-900型，美国ThermoFisher公司） 0.01mg/L 1.0% 挥发性酚 分光光度法（722G型可见分光光度计，上海仪电分析仪器有限公司） 0.0003mg/L 0.5% 
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表 2 地下水水化学组分特征
Table 2. Hydrochemistry indicators in groundwater at different depths.
水样 参数 pH 总硬度
（mg/L）TDS
（mg/L）铁
（mg/L）锰
（mg/L）铜
（mg/L）锌
（mg/L）铝
（mg/L）挥发性酚类
（mg/L）浅层 最大值 9.55 25414 91017 0.20272 3.84536 0.34050 0.37555 32.94465 0.0146 最小值 6.83 60 333 - 0.00069 - - - - 平均值 7.66 2537 8746 0.00243 0.89456 0.00832 0.02864 1.87106 0.0018 中层 最大值 9.91 25324 106387 0.01386 6.08105 21.49463 1.19925 18.97229 0.0626 最小值 6.25 18 417 - 0.00293 - - - - 平均值 8.04 2219 8112 0.00103 0.65594 0.18282 0.06215 1.47228 0.0032 深层 最大值 10.42 9359 39360 2.41837 7.38455 0.23792 0.93538 7.20163 0.0278 最小值 7.25 5 372 - 0.01223 - - - - 平均值 8.75 1300 5080 0.05886 0.70026 0.00834 0.06693 0.60395 0.0038 水样 参数 氨氮
（mg/L）氟化物
（mg/L）碘化物
（mg/L）汞
（mg/L）砷
（mg/L）铅
（mg/L）钙离子
（mg/L）镁离子
（mg/L）钾离子
（mg/L）浅层 最大值 8.10 3.78 1.920 0.07320 0.03789 0.04437 1078.67 5872.91 969.98 最小值 - 0.13 - - - - 2.75 12.21 0.32 平均值 0.29 1.25 0.332 0.00146 0.00140 0.00260 204.95 488.41 23.84 中层 最大值 9.14 13.71 1.708 0.09990 0.01193 0.67751 1117.98 5628.00 771.97 最小值 - - - - - - 1.40 3.31 0.24 平均值 0.25 1.35 0.396 0.00127 0.00060 0.00779 188.22 421.61 20.49 深层 最大值 14.26 5.28 4.601 0.29170 0.01309 0.07461 1679.83 1830.37 50.69 最小值 - - - - - - - 0.16 0.57 平均值 0.44 1.92 0.581 0.00464 0.00107 0.00248 159.83 217.25 6.71 水样 参数 类型 硫酸根
（mg/L）硝酸根
（mg/L）重碳酸根
（mg/L）类型 硫酸根
（mg/L）硝酸根
（mg/L）重碳酸根
（mg/L）浅层 平均值 正常 1342.48 12.94 598.50 高碘 2055.44 1.42 670.43 平均值 中层 正常 - - - 高碘 1513.44 1.25 381.24 平均值 深层 正常 543.98 4.57 229.15 高碘 780.41 1.65 351.70
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表 3 钻孔沉积物组分特征
Table 3. The content of each component in sediments at different depths in the two holes.
钻孔编号 深度 参数 pH 氨氮
（mg/L）氟
（mg/L）氯
（mg/L）硫酸根
（mg/L）钾
（mg/L）镁
（mg/L）钠
（mg/L）碳酸根
（mg/L）重碳酸根
（mg/L）G09 浅层 最大值 8.07 0.00272 0.02896 2.02 1.65 0.03649 0.20337 1.84 0.12 0.51 最小值 7.40 - 0.00078 0.01 0.01 0.00417 0.00471 0.02 - 0.33 平均值 7.62 0.00095 0.00599 0.80 0.57 0.01428 0.08170 0.73 - 0.42 ZK02 浅层 最大值 9.00 0.00077 0.01616 1.04 1.26 0.07529 0.07982 1.03 0.29 0.92 最小值 7.60 - 0.00280 0.09 - 0.00159 0.00457 0.20 - 0.21 平均值 8.19 0.00043 0.00745 0.46 0.56 0.00857 0.02838 0.57 0.09 0.41 中层 最大值 9.44 0.00042 0.0226 0.96 0.96 0.02731 0.04673 1.06 0.32 0.67 最小值 7.40 - 0.00187 0.11 0.10 0.00007 0.00427 0.21 - 0.15 平均值 8.49 0.00028 0.01033 0.39 0.26 0.00563 0.01391 0.47 0.13 0.40 深层 最大值 8.83 0.0006 0.02946 0.29 0.21 0.03516 0.03258 0.43 0.21 0.90 最小值 7.23 - 0.00122 0.01 0.02 0.00181 0.00239 0.07 - 0.19 平均值 7.89 0.00037 0.01099 0.09 0.07 0.00928 0.01271 0.27 0.06 0.60 注：最小值标注“-”表示低于检出限，相应的平均值也标注为“-”。
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