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S2-对河砂吸附砷的影响及其作用机理

杜海玲 单慧媚 陈辉 彭三曦 黄健

杜海玲, 单慧媚, 陈辉, 彭三曦, 黄健. S2-对河砂吸附砷的影响及其作用机理[J]. 地质科技通报, 2022, 41(4): 241-248. doi: 10.19509/j.cnki.dzkq.2022.0123
引用本文: 杜海玲, 单慧媚, 陈辉, 彭三曦, 黄健. S2-对河砂吸附砷的影响及其作用机理[J]. 地质科技通报, 2022, 41(4): 241-248. doi: 10.19509/j.cnki.dzkq.2022.0123
Du Hailing, Shan Huimei, Chen Hui, Peng Sanxi, Huang Jian. Effects of S2- on arsenic adsorption to river sand and its mechanisms[J]. Bulletin of Geological Science and Technology, 2022, 41(4): 241-248. doi: 10.19509/j.cnki.dzkq.2022.0123
Citation: Du Hailing, Shan Huimei, Chen Hui, Peng Sanxi, Huang Jian. Effects of S2- on arsenic adsorption to river sand and its mechanisms[J]. Bulletin of Geological Science and Technology, 2022, 41(4): 241-248. doi: 10.19509/j.cnki.dzkq.2022.0123

S2-对河砂吸附砷的影响及其作用机理

doi: 10.19509/j.cnki.dzkq.2022.0123
基金项目: 

国家自然科学基金项目 41877194

国家自然科学基金项目 41502232

广西自然科学基金项目 2017GXNSFAA198096

广西自然科学基金项目 2018AD19142

详细信息
    作者简介:

    杜海玲(1997-), 女, 现正攻读水利工程专业硕士学位, 主要从事地下水污染与防治研究。E-mail: 1102231518@qq.com

    通讯作者:

    单慧媚(1985-), 女, 副教授, 主要从事地下水污染与防治、水文地球化学方面的研究。E-mail: shanhuimei@glut.edu.cn

  • 中图分类号: X141

Effects of S2- on arsenic adsorption to river sand and its mechanisms

  • 摘要:

    水体中S2-与砷(As)的迁移富集密切相关, 但不同含水介质中其作用机理尚不明确。为了查明潜流带中常见含水介质河砂在S2-作用下对As的吸附特征, 设计并开展了As在河砂上的吸附动力学实验, 以及S2-作用下河砂对As的吸附实验, 结合PHREEQC模拟计算, XRD、SEM-EDS、XPS和FTIR等表征测试技术, 进一步识别其作用机理。结果表明: 固液比为25 g/L情况下, 河砂对As的吸附在200 h左右达到吸附平衡, 且对As(Ⅴ)的吸附量明显高于As(Ⅲ); 随着S2-浓度的增加, 河砂对As吸附能力逐渐减弱; 模拟及表征测试结果显示, 少量As被吸附在河砂表面, 主要与其表面的Fe、Al结合, 其中As(Ⅲ)的吸附可能还与Si-O键断裂后与S2-结合形成的SiS2有关。S2-对河砂吸附As的主要影响机理为: ①S2-的加入使得溶液pH值升高、Eh值降低, 从而抑制了As的吸附; ②添加S2-条件下河砂表面的Fe、Al等能与S和As形成AlAs、AlAsO4、FeS2及Fe4As2O11等化合物, 减少了河砂表面吸附As的活性位点。研究结果有助于丰富As-S作用机理, 以及As在地下水环境中迁移过程的认识。

     

  • 图 1  河砂对As吸附量随时间的变化曲线

    Figure 1.  Changes in As adsorption capacity of the river sand with time

    图 2  不同S2-浓度下反应平衡后溶液中As的浓度

    Figure 2.  Concentration of As in the solution after the reaction equilibrium at different S2- concentrations

    图 3  反应前后溶液中ρ(S2-)变化(其中Ⅰ、Ⅱ、Ⅲ和Ⅳ代表了ρ(S2-)初始分别为0.1, 1.0, 5.0, 20.0 mg/L的实验组)

    Figure 3.  Changes in the S2- concentration before and after the reaction (among them, Ⅰ, Ⅱ, Ⅲ and Ⅳ represent the experimental groups with S2-initial concentrations of 0.1, 1.0, 5.0, 20.0 mg/L, respectively)

    图 4  河砂反应前后的SEM-EDS图

    Figure 4.  SEM-EDS diagram of river sand before and after the reaction

    图 5  反应前后各体系河砂XRD图谱

    Figure 5.  XRD patterns of river sand before and after the reaction

    图 6  河砂反应后As3d窄谱谱图

    Figure 6.  As3d narrow spectrum of river sand after the reaction

    图 7  河砂反应前后的FTIR图谱

    Figure 7.  FTIR spectra of river sand before and after the reaction

    表  1  河砂主要成分

    Table  1.   Main composition of river sand

    成分 SiO2 Al2O3 K2O Fe2O3 CaO TiO2 MgO Na2O MnO
    wB/% 90.69 5.91 1.62 1.51 0.32 0.17 0.15 0.14 0.06
    下载: 导出CSV

    表  2  不同ρ(S2-)条件下反应前后溶液的pH和Eh对比

    Table  2.   Comparison of pH and Eh before and after the reaction at different S2- concentrations

    初始ρ(S2-)/(mg·L-1) 0.1 1.0 5.0 20.0
    As(Ⅲ) 反应前pH 7.58 9.91 10.09 11.01
    反应后pH 6.77 7.23 6.96 9.64
    反应前Eh/mV -256.40 -316.90 -338.90 -398.50
    反应后Eh/mV 223.90 174.00 115.60 -191.30
    As(Ⅴ) 反应前pH 7.22 9.24 10.28 11.01
    反应后pH 6.57 7.15 7.38 9.76
    反应前Eh/mV -283.40 -343.50 -375.10 -401.70
    反应后Eh/mV 243.93 46.93 47.6 -195.93
    下载: 导出CSV

    表  3  PHREEQC模拟中选取部分矿物饱和指数结果

    Table  3.   Selected mineral saturation index results in the PHREEQC simulation

    反应体系 ρ(S2-)/(mg·L-1) As2O3 As2O5 As2S3 AsS S
    饱和指数SI
    S2--As(Ⅲ) 0.1 -8.52 -44.05 -5.56 -1.62 -5.22
    1.0 -9.62 -45.73 -12.03 -3.81 -7.92
    5.0 -9.89 -46.7 -9.85 -3.56 -6.97
    20.0 -11.59 -48.26 -16.68 -25.12 -8.46
    S2--As(Ⅴ) 0.1 -8.74 -35.38 -59.22 -21.76 -18.58
    1.0 -9.03 -44.51 -8.87 -2.82 -6.13
    5.0 -10.24 -46.14 -12.81 -4.23 -7.25
    20.0 -11.60 -47.82 -16.71 -19.57 -8.25
    下载: 导出CSV
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出版历程
  • 收稿日期:  2021-04-27
  • 网络出版日期:  2022-09-07

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