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    高温富硫化物热泉中硫代砷化物存在形态的地球化学模拟:以云南腾冲热海水热区为例

    庄亚芹 郭清海 刘明亮 李洁祥 周超

    庄亚芹, 郭清海, 刘明亮, 李洁祥, 周超, 2016. 高温富硫化物热泉中硫代砷化物存在形态的地球化学模拟:以云南腾冲热海水热区为例. 地球科学, 41(9): 1499-1510. doi: 10.3799/dqkx.2016.513
    引用本文: 庄亚芹, 郭清海, 刘明亮, 李洁祥, 周超, 2016. 高温富硫化物热泉中硫代砷化物存在形态的地球化学模拟:以云南腾冲热海水热区为例. 地球科学, 41(9): 1499-1510. doi: 10.3799/dqkx.2016.513
    Zhuang Yaqin, Guo Qinghai, Liu Mingliang, Li Jiexiang, Zhou Chao, 2016. Geochemical Simulation of Thioarsenic Speciation in High-Temperature, Sulfide-Rich Hot Springs: A Case Study in the Rehai Hydrothermal Area, Tengchong, Yunnan. Earth Science, 41(9): 1499-1510. doi: 10.3799/dqkx.2016.513
    Citation: Zhuang Yaqin, Guo Qinghai, Liu Mingliang, Li Jiexiang, Zhou Chao, 2016. Geochemical Simulation of Thioarsenic Speciation in High-Temperature, Sulfide-Rich Hot Springs: A Case Study in the Rehai Hydrothermal Area, Tengchong, Yunnan. Earth Science, 41(9): 1499-1510. doi: 10.3799/dqkx.2016.513

    高温富硫化物热泉中硫代砷化物存在形态的地球化学模拟:以云南腾冲热海水热区为例

    doi: 10.3799/dqkx.2016.513
    基金项目: 

    中国地质大学(武汉)生物地质与环境地质国家重点实验室自主研究课题项目 GBL11505

    国家自然科学基金项目 41120124003

    国家自然科学基金项目 41572335

    国家自然科学基金项目 41521001

    详细信息
      作者简介:

      庄亚芹(1990-),女,硕士研究生,从事高温地热流体地球化学领域的研究工作.E-mail:359572236@qq.com

      通讯作者:

      郭清海, E-mail: qhguo2006@gmail.com

    • 中图分类号: P66

    Geochemical Simulation of Thioarsenic Speciation in High-Temperature, Sulfide-Rich Hot Springs: A Case Study in the Rehai Hydrothermal Area, Tengchong, Yunnan

    • 摘要: 天然水环境中地质成因砷的存在是世界范围内对人类威胁极大的环境问题之一.在高温富硫化物地热水中,硫代砷化物是砷的主要存在形态之一.在国内尚无硫代砷化物定量检测方法的背景下,以云南腾冲地热带的热海水热区为典型研究区,基于不同类型硫代砷化物的最新化学热力学数据wateq4f.dat,利用水文地球化学模拟软件PHREEQC开展了不同类型热泉中砷的存在形态的地球化学模拟.结果表明,热海热泉中砷的主要形态是硫代砷酸盐,砷酸盐和亚砷酸盐次之,硫代亚砷酸盐则含量极低;在各类硫代砷酸盐中,按平均百分含量降序依次为:一硫代砷酸盐→三硫代砷酸盐→四硫代砷酸盐→二硫代砷酸盐.pH、Eh和总硫化物含量是热泉中砷的形态分布的控制性因素.在酸性条件下,砷以硫代砷酸盐和亚砷酸盐为主要存在形式;而在中性/偏碱性条件下,砷的形态则以硫代砷酸盐为主,砷酸盐次之.偏还原环境和高硫化物含量是硫代砷化物、特别是三硫代砷酸盐和四硫代砷酸盐稳定存在的有利条件.

       

    • 图  1  腾冲火山岩分布(a)和热海热田地热地质图及采样位置(b)

      1.全新统;2.晚更新统;3.中更新统玄武岩;4.早更新统安山岩;5.中新统南林组;6.元古宙高黎贡山群;7.明矾石带;8.高岭石-玉髓或蛋白石带;9.高岭石-蒙脱石-玉髓带,高岭石-伊利石-蒙脱石混层矿物-玉髓石英带;10.伊利石-蒙脱石混层矿物-石英带;11.绿泥石-蒙脱石混层矿物带;12.蒙脱石-方解石带;13.伊利石-蒙脱石-高岭石-玉髓带;14.断层;15.取样点;16.热泉/高程(m);图a据赵慈平等(2006)修改;图b据廖志杰和赵平(1999)修改

      Fig.  1.  Volcanic rock distribution in Tengchong (a) and geothermal geological map of the Rehai field and sampling locations (b)

      图  2  基于不同氧化还原电对实测含量计算出的热泉样品Eh

      Fig.  2.  Calculated Eh values of the hot-spring samples according to the measured concentrations of various redox couples

      图  3  酸性热泉(a)和中性/偏碱性(b)热泉中砷的不同形态的百分含量随Eh、总砷浓度和总硫化物浓度的变化

      Fig.  3.  Percentage of different arsenic species vs. Eh, total arsenic, and total sulfide concentrations in acidic hot springs (a) and neutral/weak alkaline hot springs (b)

      图  4  中性/偏碱性热泉总砷浓度与Eh的关系

      Fig.  4.  Eh vs.total arsenic concentration in neutral/weak alkaline hot springs

      图  5  控制条件下砷的形态分布与总砷含量的关系

      Fig.  5.  Relationship between arsenic speciation and total arsenic concentration under controlled conditions

      图  6  不同形态硫代砷酸盐百分含量与Eh和总硫化物浓度的关系

      Fig.  6.  Percentage of mono-, di-, tri-and tetra-thioarsenates vs. Eh (a) and total sulfide concentration (b) in all hot springs

      表  1  热海热泉的水化学组成

      Table  1.   Hydrochemical compositions of hot springs from the Rehai geothermal field

      水样编号 泉名 T pH Eh SO4 Cl F NO3 Na K Ca Mg Fe(Ⅱ) Fe(Ⅲ) As(Ⅴ) As(Ⅲ) As 硫化物 NH4
      酸性泉
      DRTY-01 地热体验区1号泉 41.6 1.85 229.8 882.7 22.8 0.5 3.5 9.9 26.2 3.3 0.7 1.94 3.70 30.9 6.8 26.0 0.01 0.4
      DRTY-02 地热体验区2号泉 65.4 1.85 199.8 776.1 22.6 0.7 4.5 4.2 4.6 8.4 0.9 1.22 2.30 35.1 7.1 35.9 0.02 3.2
      DRTY-04 地热体验区4号泉 68.7 1.93 196.4 879.0 24.8 1.4 5.0 18.0 35.4 3.5 1.2 5.69 12.60 120.2 16.3 147.8 0.02 1.6
      DRTY-06 地热体验区6号泉 85.4 2.04 168.1 1 634.0 22.9 0.5 5.1 5.6 20.0 3.5 1.1 2.64 7.70 108.6 9.0 98.2 0.03 13.5
      DRTY-07 地热体验区7号泉 80.4 1.41 185.6 1 699.6 23.3 1.3 3.9 11.3 35.8 3.7 2.4 2.60 16.30 113.6 32.3 158.6 0.04 14.3
      ZZQ-R 珍珠泉-右 86.8 2.96 128.5 135.1 41.9 1.4 0.2 56.4 26.5 2.1 0.5 0.03 0.51 11.7 47.0 62.8 0.03 6.0
      ZZQ-C 珍珠泉-出 89.0 2.81 119.9 235.9 35.9 0.8 1.2 54.6 28.8 3.6 0.7 0.07 0.87 26.4 32.1 62.8 0.04 5.4
      DGG-AS 大滚锅酸性泉 49.3 2.08 199.4 1 506.9 32.0 1.8 3.6 55.5 18.2 178.3 52.6 3.75 48.00 20.9 5.9 22.8 0.07 0.0
      LGG-HT 老滚锅(高温) 66.1 2.73 160.6 653.8 58.1 2.6 3.6 161.1 29.4 10.1 1.8 0.56 0.58 12.6 17.9 27.9 0.02 0.0
      中性/偏碱性泉
      ZZQ-L 珍珠泉-左 90.1 5.10 -6.1 162.2 42.5 2.0 1.6 64.4 30.2 2.3 0.5 0.16 0.35 21.0 44.0 62.7 0.01 3.8
      YJQ-C 眼镜泉汇 66.3 9.47 -404.6 34.0 561.7 14.7 3.0 793.8 139.7 1.0 0.1 0.01 0.00 107.4 597.6 958.8 0.35 0.1
      YJQ-L 眼镜泉左 91.1 8.88 -435.3 33.1 594.0 15.3 2.9 771.0 133.8 1.2 0.1 0.00 0.03 31.6 574.8 347.8 3.40 0.3
      YJQ-R 眼镜泉右 81.1 9.32 -439.8 33.7 612.0 15.6 3.0 786.0 136.6 1.0 0.1 0.00 0.02 49.7 628.4 768.8 2.60 0.2
      ZXS 忠孝寺泉 46.3 6.09 -95.5 35.8 134.1 3.2 2.9 253.1 47.6 17.9 1.1 0.01 0.13 136.5 20.3 129.0 0.01 0.1
      ZT07 澡塘河仙人澡塘 46.0 7.60 -180.4 73.2 236.8 7.5 2.9 369.6 66.7 7.6 0.3 0.28 0.00 86.4 161.5 267.4 0.04 0.2
      DGG-NS 大滚锅 84.1 7.45 -334.4 40.3 715.9 19.2 2.8 893.4 153.6 1.0 0.1 0.03 0.01 940.6 104.6 548.9 0.21 0.0
      HMZT-M 蛤蟆嘴亭中 57.5 7.40 -189.5 72.0 288.8 7.0 4.2 372.2 66.8 4.7 0.7 0.40 0.04 71.2 173.7 271.3 0.06 0.0
      HMZT-L 蛤蟆嘴亭左 64.2 7.14 -213.1 63.7 332.0 8.1 4.6 420.9 76.5 3.6 0.5 0.45 0.01 115.3 249.3 425.5 0.13 0.0
      HMZD 蛤蟆嘴池 91.6 7.13 -319.7 43.9 337.6 8.0 4.4 449.7 81.9 2.3 0.2 0.06 0.00 123.2 124.7 290.8 0.30 0.0
      XKT-R 霞客亭右 95.0 7.53 -229.8 37.3 335.6 8.0 4.2 456.1 81.4 2.2 0.1 0.02 0.00 79.4 146.7 293.0 1.90 0.0
      HTJ-L 怀胎井左 92.4 7.40 -385.1 33.3 560.7 13.8 4.2 692.6 124.5 1.0 0.1 0.00 0.02 127.9 461.4 573.8 2.60 0.0
      HTJ-R 怀胎井右 85.4 6.88 -317.2 44.5 464.6 11.5 3.9 547.6 100.1 1.4 0.1 0.02 0.00 403.6 151.3 657.4 0.67 0.0
      GMQ 鼓鸣泉 90.5 8.12 -424.2 32.2 593.9 14.5 4.2 716.2 127.9 1.3 0.1 0.01 0.01 50.7 346.9 314.6 5.00 0.0
      TQL 听泉楼 82.3 7.96 -394.0 31.1 597.1 14.6 3.9 699.0 113.1 1.0 0.1 0.01 0.00 78.8 398.8 278.4 3.00 0.0
      注:T的单位为℃;Eh的单位为mV;As(Ⅴ)、As(Ⅲ)和As的单位为μg/L;其他化学组分的单位为mg/L.
      下载: 导出CSV

      表  2  砷的不同形态的化学热力学数据

      Table  2.   Chemical thermodynamic data of arsenic species

      砷的形态 化学结构式 化学反应式 lgK 来源
      亚砷酸盐 HnAsO3n-3 H3AsO3=H2AsO3-+H+ -9.15 Parkhurst and Appelot (1999)
      H2AsO3-=HAsO32-+H+ -23.85 Parkhurst and Appelot (1999)
      HAsO32-=AsO33-+H+ -39.55 Parkhurst and Appelot (1999)
      一硫代亚砷酸盐 HnAsSO2n-3 H3AsO3+H2S=H3AsSO2+H2O 0.4 Helz and Tossell (2008)
      H3AsSO2=H2AsSO2-+H+ -3.8 Zaksznova-Herzog and Seward(2012)
      H2AsSO2-=HAsSO22-+H+ ≤-13.5 Zaksznova-Herzog and Seward(2012)
      HAsSO22-=AsSO23-+H+ ≤-14.0 Zaksznova-Herzog and Seward(2012)
      二硫代亚砷酸盐 HnAsS2On-3 H3AsSO2+H2S=H3AsS2O+H2O 3.8 Helz and Tossell (2008)
      H3AsS2O=H2AsS2O-+H+ -3.8 Zaksznova-Herzog and Seward(2012)
      H2AsS2O-=HAsS2O2-+H+ -6.5 Zaksznova-Herzog and Seward(2012)
      HAsS2O2-=AsS2O3-+H+ -14.0 Zaksznova-Herzog and Seward(2012)
      三硫代亚砷酸盐 HnAsS3n-3 H3AsS2O+H2S=H3AsS3+H2O 5.6 Helz and Tossell(2008)
      H3AsS3=H2AsS3-+H+ -3.77 Zaksznova-Herzog and Seward(2012)
      H2AsS3-= HAsS32-+H+ -6.53 Zaksznova-Herzog and Seward(2012)
      HAsS32-=AsS33-+H+ -9.29 Zaksznova-Herzog and Seward(2012)
      砷酸盐 HnAsO4n-3 H3AsO4=H2AsO4-+H+ -2.3 Parkhurst and Appelot (1999)
      H2AsO4-=HAsO42-+H+ -9.46 Parkhurst and Appelot (1999)
      HAsO42-=AsO43-+H+ -21.11 Parkhurst and Appelot (1999)
      一硫代砷酸盐 HnAsSO3n-3 H3AsO4+H2S=H3AsSO3+H2O 11.0 Helz and Tossell(2008)
      H3AsSO3=H2AsSO3-+H+ -3.3 Thilo et al.(2004)
      H2AsSO3-= HAsSO32-+H+ -7.2 Thilo et al.(2004)
      HAsSO32-= AsSO3-3+H+ -11.0 Thilo et al.(2004)
      二硫代砷酸盐 HnAsS2O2n-3 H3AsSO3+H2S=H3AsS2O2+H2O 0.1 Helz and Tossell (2008)
      H3AsS2O2=H2AsS2O2-+H+ 2.4 Helz and Tossell (2008)
      H2AsS2O2-=HAsS2O22-+H+ -7.1 Thilo et al.(2004)
      HAsS2O22-= AsS2O2-3+H+ -10.8 Thilo et al.(2004)
      三硫代砷酸盐 HnAsS3On-3 H3AsS2O2+H2S=H3AsS3O+H2O 3.5 Helz and Tossell (2008)
      H3AsS3O=H2AsS3O-+H+ 1.7 Helz and Tossell (2008)
      H2AsS3O-= HAsS3O2-+H+ -1.5 Helz and Tossell (2008)
      HAsS3O2-= AsS3O3-+H+ -10.8 Thilo et al.(2004)
      四硫代砷酸盐 HnAsS4n-3 H3AsS3O+H2S=H3AsS4+H2O 2.6 Helz and Tossell (2008)
      H3AsS4=H2AsS4-+H+ 2.3 Helz and Tossell (2008)
      H2AsS4-=HAsS42-+H+ -1.5 Helz and Tossell (2008)
      HAsS42-= AsS43-+H+ -5.2 Thilo et al.(2004)
      下载: 导出CSV

      表  3  热泉中各种硫代砷化物的含量

      Table  3.   Concentrations of different thioarsenate in the hot springs

      样品编号 亚砷酸盐 砷酸盐 硫代亚砷酸盐 硫代砷酸盐 总砷(μg /L) 一硫代砷酸盐 二硫代砷酸盐 三硫代砷酸盐 四硫代砷酸盐
      (μg/L) % (μg/L) % (μg/L) % (μg/L) % (μg/L) % (μg/L) % (μg/L) % (μg/L) %
      DRTY-01 2.54E+01 97.96 2.42E-05 0.000 1.99E-05 0.000 5.28E-01 2.04 25.91 0.52 98.95 0.01 1.04 0.00 0.00 0.00 0.00
      DRTY-02 1.99E+01 55.56 5.11E-04 0.001 2.10E-05 0.000 1.59E+01 44.44 35.86 15.71 98.61 0.22 1.39 0.00 0.00 0.00 0.00
      DRTY-04 1.10E+02 74.28 4.29E-03 0.003 3.28E-05 0.000 3.79E+01 25.71 147.50 37.77 99.60 0.15 0.40 0.00 0.00 0.00 0.00
      DRTY-06 3.34E+01 33.98 1.22E-02 0.012 6.01E-06 0.000 6.49E+01 66.01 98.31 64.71 99.73 0.18 0.27 0.00 0.00 0.00 0.00
      DRTY-07 7.22E+01 45.53 1.19E-02 0.008 1.74E-05 0.000 8.64E+01 54.46 158.65 86.12 99.66 0.29 0.34 0.00 0.00 0.00 0.00
      ZZQ-R 2.28E-01 0.36 1.96E-02 0.031 5.65E-08 0.000 6.26E+01 99.61 62.89 61.53 98.23 1.10 1.76 0.00 0.00 0.00 0.00
      ZZQ-C 8.85E-02 0.14 3.82E-03 0.006 8.96E-08 0.000 6.28E+01 99.85 62.89 59.22 94.30 3.56 5.67 0.02 0.04 0.00 0.00
      DGG-AS 1.35E+01 59.17 6.14E-05 0.000 7.31E-05 0.000 9.31E+00 40.83 22.80 8.55 91.83 0.75 8.09 0.01 0.08 0.00 0.00
      LGG-HT 1.35E+00 4.83 2.49E-03 0.009 9.40E-07 0.000 2.66E+01 95.16 27.96 25.63 96.35 0.97 3.63 0.00 0.02 0.00 0.00
      ZZQ-L 1.58E-04 0.000 3.94E+01 62.74 3.22E-13 0.000 2.34E+01 37.26 62.79 23.39 100.00 0.00 0.00 0.00 0.00 0.00 0.00
      YJQ-C 5.30E-17 0.000 4.90E+02 50.92 5.94E-22 0.000 4.72E+02 49.08 962.30 472.28 99.99 0.03 0.01 0.00 0.00 0.00 0.00
      YJQ-L 2.19E-18 0.000 3.04E+00 0.87 1.28E-21 0.000 3.46E+02 99.13 349.09 336.98 97.38 2.46 0.71 5.59 1.62 1.02 0.29
      YJQ-R 3.50E-18 0.000 4.67E+01 6.05 4.09E-22 0.000 7.25E+02 93.95 771.63 723.88 99.86 0.77 0.11 0.25 0.03 0.02 0.00
      ZXS 8.33E-05 0.000 1.06E+02 81.89 8.64E-13 0.000 2.34E+01 18.11 129.25 23.41 100.00 0.00 0.00 0.00 0.00 0.00 0.00
      ZT07 8.97E-10 0.000 1.74E+02 65.10 7.90E-16 0.000 9.35E+01 34.90 268.03 93.53 100.00 0.00 0.00 0.00 0.00 0.00 0.00
      DGG-NS 7.75E-12 0.000 6.03E+01 10.93 6.09E-17 0.000 4.91E+02 89.07 551.15 490.62 99.94 0.24 0.05 0.03 0.01 0.00 0.00
      HMZT-M 7.86E-10 0.000 1.32E+02 48.45 8.12E-16 0.000 1.40E+02 51.55 271.94 140.18 99.99 0.01 0.01 0.00 0.00 0.00 0.00
      HMZT-L 2.68E-09 0.000 1.22E+02 28.66 3.44E-15 0.000 3.04E+02 71.34 426.56 304.27 99.98 0.05 0.02 0.00 0.00 0.00 0.00
      HMZD 1.37E-13 0.000 1.43E-01 0.05 6.56E-17 0.000 2.91E+02 99.95 291.57 158.50 54.39 9.29 3.19 120.57 41.37 3.06 1.05
      XKT-R 9.49E-19 0.000 4.01E-05 0.00 1.84E-20 0.000 2.94E+02 100.00 293.78 0.64 0.22 0.59 0.20 148.51 50.55 144.03 49.03
      HTJ-L 9.01E-19 0.000 1.07E-05 0.00 2.99E-20 0.000 5.76E+02 100.00 575.75 0.31 0.05 0.52 0.09 229.58 39.88 345.33 59.98
      HTJ-R 2.82E-12 0.000 2.02E-01 0.03 1.08E-15 0.000 6.59E+02 99.97 659.35 304.61 46.21 23.36 3.54 324.55 49.24 6.63 1.01
      GMQ 2.72E-19 0.000 1.06E-03 0.00 4.37E-21 0.000 3.16E+02 100.00 315.71 4.92 1.56 1.46 0.46 132.25 41.89 177.06 56.08
      TQL 7.50E-19 0.000 3.34E-04 0.00 1.52E-20 0.000 2.79E+02 100.00 279.36 2.19 0.78 0.94 0.34 119.58 42.80 156.66 56.08
      注:百分比为相对于总砷浓度的百分含量.
      下载: 导出CSV
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