Migration and Transformation Mechanism of High Arsenic Groundwater in Oasis Belt in Middle Part of Northern Piedmont of Tianshan Mountain
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摘要: 准噶尔盆地是典型高砷地下水分布的内陆盆地，地下水作为盆地重要饮用水源，区域供水安全存在风险，高砷地下水迁移转化规律有待进一步查明. 以天山北麓中段绿洲带为研究区，采用半变异函数模型和UNMIX源解析模型分析该区地下水砷的分布、地下水化学组分源贡献；结合地质条件、赋存环境与水文地球化学作用剖析典型剖面高砷地下水中砷的迁移转化与富集影响因素. 结果表明：研究区地下水整体为弱碱性、偏还原环境的淡水，As含量在ND~887.0 μg·L-1之间，平均值为11.2 μg·L-1，ρ（As） > 10 μg·L-1的高砷地下水水化学类型以HCO3·SO4·Cl⁃Na（HSL⁃N型）和HCO3·SO4⁃Na（Na·Ca）型（HS-N（NC）型）为主. 单一结构潜水、承压水区潜水、承压水中高砷地下水占比分别为0.4%、6.4%、18.6%，高砷地下水主要富集于冲积平原深度100~300 m的承压含水层中. 原生矿物源、岩盐矿物源、土壤输入‒人为排放源、硫酸‒碳酸岩盐矿物源和环境影响源对地下水水化学组分贡献率分别为11.3%、21.1%、23.1%、23.4%和21.1%. 25组典型剖面地下水样中，24组地下水砷形态为As（Ⅴ）（占取样点的96.0%）. 沿着地下水流向，从山前倾斜平原到冲积平原，地下水总As含量呈先增大后减小的变化趋势. 地下水砷富集不仅受到赋存环境中pH、Eh、HCO3-和PO43-等水化学指标的影响，还与地质条件、水文地质条件、有机质降解和溶滤作用等因素有关.Abstract: Junggar Basin is a typical inland basin with high arsenic groundwater distribution. Groundwater is an important drinking water source in the basin. Regional water supply safety is at risk. Migration and transformation of high arsenic groundwater need to be further investigated. In this study, the oasis belt in the middle part of the northern piedmont of Tianshan Mountain was taken as the research area. Semivariogram model and UNMIX source analysis model were used to analyze the distribution of arsenic in groundwater and the source contribution rate of groundwater chemical indexes, and influencing factors of arsenic migration. Transformation and enrichment in high arsenic groundwater in the typical profile were analyzed in combination with geological conditions, occurrence environment and hydrogeochemical action. Results show that groundwater in the study area is generally freshwater with weak alkaline and slightly reduced environment. Groundwater As concentration ranges between ND and 887.0 μg·L-1, with an average of 11.2 μg·L-1. Hydrochemical types of high arsenic groundwater (ρ (As) > 10 μg·L-1) are mainly HCO3·SO4·Cl⁃Na (HSL⁃N) and HCO3·SO4⁃Na (Na·Ca) (HS⁃N (NC)) types. Proportions of high arsenic groundwater in single-structure phreatic water, phreatic water in confined water area, and confined water are 0.4%, 6.4%, and 18.6%, respectively. Contribution rates of native mineral source, rock salt mineral source, soil input-human emission source, sulfuric-carbonate mineral source and environmental source to groundwater hydrochemical indexes are 11.3%, 21.1%, 23.1%, 23.4% and 21.1%, respectively. Arsenic species in 24 groups of a total of 25 groundwater samples of typical profiles is only As (Ⅴ) (96.0% of the sampling sites). From piedmont plain to alluvial plain, along groundwater flow, the variation trend of groundwater total arsenic concentration firstly increased and then decreased. Arsenic enrichment in occurrence environment is affected by groundwater hydrochemical indexes including pH, Eh, HCO3- and PO43-, which is also related to geological, hydrogeological conditions, organic matter degradation, and dissolution.
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图 2 基于地下水砷分类的Drove图
Fig. 2. Drove diagram based on arsenic classification in groundwater
图 4 南北向典型剖面地下水中As与相关指标含量沿程变化
图中水化学指标pH为无量纲，∑As、As（Ⅴ）和硫化物单位为μg·L-1，Eh单位为mV，其余为mg·L-1；$ \frac{\mathrm{G}1}{\mathrm{H}\mathrm{S}\mathrm{-}\mathrm{N}\mathrm{C}} $表示$ \frac{\mathrm{编}\mathrm{号}}{\mathrm{水}\mathrm{化}\mathrm{学}\mathrm{类}\mathrm{型}} $；水化学类型中H、S、L、C、M和N分别表示HCO3、SO4、Cl、Ca、Mg和Na
Fig. 4. Variation of As and related index concentration in groundwater along the typical north-south profile
图 5 潜水（a、b、c、d）和承压水（e、f、g、h）中As、pH、TDS和Eh的水平分布
Fig. 5. Horizontal distribution of As, pH, TDS and Eh in unconfined groundwater (a, b, c, d) and confined groundwater (e, f, g, h)
图 6 地下水中As (a)、pH (b)、TDS (c)和Eh (d)的垂向分布
Fig. 6. Vertical distribution of As (a), pH (b), TDS (c) and Eh (d) in groundwater
图 7 UNMIX模型中各个因子贡献百分比（a），各水化学指标的因子图谱（b），各指标之间相关性和因子之间的联系（c）
Fig. 7. Contribution of each factor in UNMIX model (a), contribution of each hydrochemistry index to factor (b), correlations between each index and relationship between each index and factors (c)
图 8 研究区第四纪地质图(改自王彩华, 2005）
Fig. 8. Quaternary geological map of the study area (modified from Wang, 2005)
图 9 南北剖面地下水As与γCa2+/γCl-的关系
Fig. 9. Relationship between As and γCa2+/γCl- in groundwater in north-south section
图 10 地下水中砷化物含量（a）和主要矿物相的饱和指数(SI)（b）
Fig. 10. Arsenide concentration (a) and saturation index (SI) of main mineral phases (b) in groundwater
图 11 高砷地下水As与DOC（a）、DIC（b）的关系，DIC与DOC（c）、HCO3-（d）的关系
Fig. 11. Relationship between As and DOC (a), DIC (b) and relationship between DIC and DOC (c), HCO3- (d) in high arsenic groundwater
图 12 高砷地下水As与HCO3-（a）、PO3-（b）、DO（c）和γSO42-/γCl-（d）的关系
Fig. 12. Relationship between As and HCO3- (a), PO3- (b), DO (c), γSO42-/γCl- (d) in high arsenic groundwater
图 13 南北向典型剖面地下水水化学和砷形成过程
Fig. 13. Groundwater hydrochemistry and arsenic formation process in the north-south typical profile
表 1 典型剖面高砷与低砷地下水中的水化学指标对比
Table 1. Comparison of hydrochemistry indexes in high arsenic and low-arsenic groundwater in typical profiles
地下水As含量水平 特征值 ∑As As(Ⅲ) As(Ⅴ) pH DO Eh TDS DIC DOC PO43- HCO3- NO3- 硫化物 TFe 高砷地下水（n=17） 最小值 12.5 0 12.5 8.2 0.35 30.1 164.5 13.54 0.29 0.04 85.46 0.15 2.0 ND 最大值 42.6 14.8 42.3 9.2 4.52 319.0 1 474.7 29.33 1.80 0.35 163.60 4.88 72.0 0.07 平均值 25.4 0.9 24.5 8.7 1.97 160.2 484.9 19.81 0.79 0.17 117.59 0.60 20.0 0.06 低砷地下水（n=8） 最小值 0.5 0 0.5 7.6 0.63 33.3 220.7 15.28 0.37 0.04 101.33 2.08 4.0 ND 最大值 7.2 0 7.2 8.4 2.96 480.3 3 028.4 120.17 1.76 0.31 629.98 21.14 66.0 0.27 平均值 3.2 0 3.2 8.1 1.77 255.4 1 130.9 36.32 0.84 0.09 275.92 4.77 16.5 0.27 注：n为样本数；水化学指标中pH为无量纲，∑As、As(Ⅲ)、As(Ⅴ)和硫化物的单位为μg·L-1，Eh单位为mV，其余为mg·L-1. 
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表 2 地下水中As、pH和TDS半方差模型特征参数
Table 2. Characteristic parameters of As, pH and TDS semivariance model in groundwater
地下水类型 化学组分 理论模型 块金值C0 基台值C0+C 块金系数C0/(C0+C)(%) 变程(km) R2 RSS 潜水 As 球状模型 0.50 1.41 35.5 52.40 0.82 0.21 pH 指数模型 0.14 0.28 50.0 79.50 0.79 2.18×10-3 TDS 指数模型 3.0×10‒4 1.0×10‒3 30.0 51.90 0.76 1.39×10‒6 Eh 线性模型 6 515.11 6 515.11 100.0 90.28 0.69 1.35×107 承压水 As 高斯模型 0.02 0.03 66.7 70.84 0.83 7.95×10‒5 pH 指数模型 0.18 0.37 48.6 66.60 0.65 5.49×10‒3 TDS 指数模型 2.0×10‒4 3.85×10‒3 5.2 234.60 0.54 4.56×10‒9 Eh 指数模型 4 570 14 140 32.3 80.10 0.87 5.29×106
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表 3 南北剖面不同地下水类型中砷和各指标含量统计
Table 3. Statistics of arsenic and index concentration in different groundwater types in the north-south section
地下水类型 地下水As含量水平 编号/特征值 ∑As As(Ⅲ) As(Ⅴ) pH DO Eh TDS DIC DOC PO43- HCO3- NO3- 硫化物 TFe 单一结构潜水 低砷地下水(n=2) G1 0.5 ND 0.5 8.2 2.96 438.6 316.0 26.76 0.37 0.04 170.00 5.38 66.0 ND G2 1.2 ND 1.2 7.9 2.85 480.3 1 029.3 39.64 0.42 0.31 218.54 15.75 10.0 ND 平均值 0.9 ND 0.9 8.1 2.91 459.5 672.7 33.20 0.40 0.18 194.27 10.57 38.0 ND 承压水区潜水 低砷地下水(n=3) 最小值 1.2 ND 1.2 7.6 0.90 108.1 220.7 18.00 0.85 0.04 108.66 2.08 4.0 ND 最大值 6.8 ND 6.8 8.2 2.81 384.5 3 028.4 111.08 1.76 0.07 540.85 3.50 17.0 0.27 平均值 3.5 ND 3.5 7.9 1.61 246.5 1 498.9 50.29 1.15 0.05 258.42 2.60 9.0 ND 承压水 低砷地下水(n=2) G12 7.2 ND 7.2 8.4 0.63 33.3 1 274.7 21.69 1.05 0.08 137.96 2.17 6.0 ND G13 3.2 ND 3.2 8.2 1.53 86.2 2 237.0 120.17 1.42 0.10 629.98 21.14 14.0 ND 平均值 5.2 ND 5.2 8.3 1.08 59.8 1 755.9 70.93 1.24 0.09 383.97 11.66 10.0 ND 高砷地下水(n=6) 最小值 29.9 ND 29.9 8.7 1.62 63.6 367.6 23.16 0.57 0.26 94.01 0.15 4.0 ND 最大值 38.9 ND 38.9 9.2 3.57 135.2 1 474.7 29.33 1.11 0.35 163.60 4.88 72.0 0.07 平均值 33.8 ND 33.8 8.9 2.28 103.0 787.9 25.72 0.85 0.31 127.99 1.73 23.5 ND 注：n为样本数；水化学指标中pH为无量纲，∑As、As(Ⅲ)、As(Ⅴ)和硫化物单位为μg·L-1，Eh单位为mV，其余为mg·L-1.
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表 4 南北向剖面地下水反向水文地球化学模拟结果
Table 4. Reverse hydrogeochemical simulation results in groundwater of the north-south profile
矿物相 （单一结构潜水）G1→G2 （承压水）G5→G7 （承压水）G10→G12 方解石（CaCO3） 3.28×10‒4 ‒3.64×10‒4 ‒ 白云石（CaMg(CO3)2） 3.28×10‒4 1.41×10‒4 -6.36×10‒5 石膏（CaSO4·2H2O） 3.33×10‒3 -1.18×10‒4 2.41×10‒3 岩盐（NaCl） 3.18×10‒3 -1.96×10‒4 9.55×10‒3 雌黄（As2S3） -2.35×10‒6 -2.33×10‒7 4.85×10‒7 雄黄（AsS） 4.70×10‒6 5.25×10‒7 -1.39×10‒6 CO2(g) 3.63×10‒4 1.22×10‒4 -2.82×10‒3 NaX -1.53×10‒3 6.02×10‒4 1.27×10‒3 CaX2 - - -1.35×10‒3 MgX2 7.67×10‒4 -3.01×10‒4 7.17×10‒4 注：表中正值表示溶解，负值表示沉淀，“-”表示未参加反应.
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