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    流速及介质粒径对As(Ⅲ)迁移影响的实验研究

    杜海玲 单慧媚 黄健 曾春芽 张进贤 刘允全

    杜海玲, 单慧媚, 黄健, 曾春芽, 张进贤, 刘允全, 2024. 流速及介质粒径对As(Ⅲ)迁移影响的实验研究. 地球科学, 49(4): 1459-1469. doi: 10.3799/dqkx.2022.316
    引用本文: 杜海玲, 单慧媚, 黄健, 曾春芽, 张进贤, 刘允全, 2024. 流速及介质粒径对As(Ⅲ)迁移影响的实验研究. 地球科学, 49(4): 1459-1469. doi: 10.3799/dqkx.2022.316
    Du Hailing, Shan Huimei, Huang Jian, Zeng Chunya, Zhang Jinxian, Liu Yunquan, 2024. Experiment on Influence of Flow Velocity and Medium Particle Size on As(Ⅲ) Migration. Earth Science, 49(4): 1459-1469. doi: 10.3799/dqkx.2022.316
    Citation: Du Hailing, Shan Huimei, Huang Jian, Zeng Chunya, Zhang Jinxian, Liu Yunquan, 2024. Experiment on Influence of Flow Velocity and Medium Particle Size on As(Ⅲ) Migration. Earth Science, 49(4): 1459-1469. doi: 10.3799/dqkx.2022.316

    流速及介质粒径对As(Ⅲ)迁移影响的实验研究

    doi: 10.3799/dqkx.2022.316
    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 2167026

    广西自然科学基金项目 2022GXNSFBA035600

    详细信息
      作者简介:

      杜海玲(1997-),女,硕士研究生,主要研究方向为地下水污染与防治.ORCID:0000-0002-7534-5025. E-mail:1102231518@qq.com

      通讯作者:

      单慧媚,女,教授,主要从事水污染与防治和水文地球化学研究. E-mail:shanhuimei@glut.edu.cn

    • 中图分类号: P641

    Experiment on Influence of Flow Velocity and Medium Particle Size on As(Ⅲ) Migration

    • 摘要: 为了解潜流带中地下水流速和介质颗粒对As(Ⅲ)迁移的影响,选用天然河砂为介质,配制地下水含As(Ⅲ)模拟液,开展室内批实验和动态柱实验并进行表征分析,探讨流速和介质粒径对As(Ⅲ)迁移的影响及机制.结果发现:(1)粒径越小的河砂与As(Ⅲ)相互作用平衡时间越长,As(Ⅲ)的单位吸附量(Qe)随着河砂粒径的增大而减小(0.15~0.18 mm的粒径河砂除外),单层最大吸附量(Qm)随着粒径的增大呈减小趋势;(2)As(Ⅲ)在河砂上的迁移行为表现出明显的粒径和流速效应;一方面,河砂粒径越小,比表面积越大,增加了水-砂相互作用时间和限制了地下水冲洗速度,不利于As(Ⅲ)在河砂中的迁移;另一方面,流速越大导致空隙通道内的水力剪切力增强,紊流强度的提高减小了滞留边界层厚度,利于As(Ⅲ)在河砂中的迁移.

       

    • 图  1  实验装置示意图

      Fig.  1.  Schematic diagram of device experiments

      图  2  河砂对As(Ⅲ)的吸附动力学曲线

      Fig.  2.  The curves of the adsorption of As(Ⅲ) with time

      图  3  河砂吸附As(Ⅲ)的动力学拟合

      Fig.  3.  Kinetic fitting of arsenic (Ⅲ) adsorption by river sand

      图  4  河砂对As(Ⅲ)的吸附等温线

      Fig.  4.  Adsorption isotherm for As(Ⅲ) adsorption on river sand

      图  5  0.377 cm/min(a)和0.754 cm/min(b)流速下,不同粒径砂柱中As(Ⅲ)的穿透曲线

      Fig.  5.  Breakthrough curve of As(Ⅲ) on river sand with different particle size at flow rates of 0.377 cm/min (a) and 0.754 cm/min (b)

      图  6  As(Ⅲ)在不同流速下的穿透曲线

      Fig.  6.  Breakthrough curve of As(Ⅲ) at different flow rates

      图  7  河砂(0.08~0.15 mm)吸附前后的SEM和EDS图

      图中,a1、b1和c1对应于a、b和c的EDS图

      Fig.  7.  SEM image and EDS mapping of river sand (0.08-0.15 mm) before and after adsorption

      图  8  河砂(0.08~0.15 mm)吸附前后XRD谱图和FTIR图

      Fig.  8.  XRD pattern (a) and FTIR spectra (b) of river sand (0.08-0.15 mm) before and after adsorption

      表  1  河砂及模拟液主要成分

      Table  1.   Main components of river sand and simulated liquid

      河砂 含量(%) 模拟液 浓度(mg/L) 模拟液 浓度及特性
      SiO2 90.69 DO < 2 CO32-(mg/L) -
      Al2O3 5.91 K+ 0.312 pH 8.27
      K2O 1.62 Ca2+ 59.53 Eh(mV) 253.7
      Fe2O3 1.51 Na+ 4.18 EC(μS/cm) 254
      CaO 0.32 Mg2+ 7.61
      TiO2 0.17 Cl 9.52
      MgO 0.15 NO3 3.54
      Na2O 0.14 SO42- 15.66
      MnO 0.06 HCO3 179.7
      下载: 导出CSV

      表  2  各砂柱实验参数

      Table  2.   Sand column experimental parameters

      流速(cm/min) 粒径(mm) 孔隙体积(cm3) 河砂质量(g) 平均比表面积(m2/g)
      0.377/0.754 0.25~1.00 29.0 133.071 9 0.641
      0.18~0.25 27.5 128.468 1 1.174
      0.08~0.15 22.0 123.781 7 1.396
      下载: 导出CSV

      表  3  动力学吸附模型

      Table  3.   Kinetic sorption models

      模型名称 方程 模型参数 参考文献
      准一级动力学 $ {Q}_{\mathrm{t}}={Q}_{\mathrm{e}}(1-{\mathrm{e}}^{-{K}_{1}t}) $ 一级吸附速率常数(K1) Lagergren(1898)
      平衡吸附量(Qe)
      准二级动力学 Qt=$ \frac{{Q}_{\mathrm{e}}^{2}{K}_{2}t}{1+{Q}_{\mathrm{e}}{K}_{2}t} $ 二级吸附速率常数(K2) Ho and McKay(1999)
      颗粒内扩散模型 $ {Q}_{\mathrm{t}}={K}_{1}{t}^{\frac{1}{2}}+C $ 内扩散速率常数(KI) Jr Weber and Morris(1963)
      常量(C)
      Elovich QtIn(αβ)+βIn(t) 常量(β) Low(1960)
      常量(α)
      Freundlich $ {Q}_{\mathrm{e}}={K}_{\mathrm{F}}{C}_{\mathrm{e}}^{\frac{1}{n}} $ 吸附能力相关常数(KF) Namasivayam and Senthilkumar(1998)
      吸附能相关常数(n)
      Langmuir Qe=$ \frac{{Q}_{\mathrm{m}}{K}_{\mathrm{L}}{C}_{\mathrm{e}}}{1+{K}_{\mathrm{L}}{C}_{\mathrm{e}}} $ 吸附能相关常数(KL) Langmuir(1918)
      吸附平衡时吸附质的质量浓度(Ce)
      下载: 导出CSV

      表  4  河砂对As(Ⅲ)的吸附动力学拟合参数

      Table  4.   Kinetic parameters for As(Ⅲ) adsorption on river sand

      模型 参数 粒径(mm)
      1.00~2.00 0.25~1.00 0.18~0.25 0.15~0.18 0.08~0.15
      准一级动力学 Qe(µg/g) 13.647 12.260 15.921 16.201 18.677
      K1 0.024 0.092 0.041 0.017 0.010
      R2 0.871 0.924 0.584 0.925 0.954
      准二级动力学 Qe(µg/g) 14.902 14.127 12.666 17.447 23.054
      K2 0.002 0.006 0.034 0.002 0.000
      R2 0.898 0.943 0.687 0.942 0.964
      颗粒内扩散模型 C 3.286 2.295 2.372 2.256 1.623
      KI 0.582 0.880 0.837 0.778 0.908
      R2 0.930 0.991 0.992 0.982 0.987
      Elovich β 2.158 5.315 5.508 4.293 7.305
      α 0.684 0.012 0.012 0.030 0.004
      R2 0.906 0.990 0.992 0.989 0.988
      下载: 导出CSV

      表  5  Langmuir和Freundlich等温吸附模型拟合参数

      Table  5.   Fitting parameters by Langmuir isotherm and Freundlich isotherm models

      粒径(mm) Langmuir Freundlich
      KL(10-4 L/g) Qm(µg/g) R2 KF/(mg1-1/n·L1/n·g-1) n R2
      1.00~2.00 0.082 140.350 0.967 24.048 2.427 0.940
      0.25~1.00 0.070 149.875 0.824 32.154 2.972 0.757
      0.18~0.25 0.062 158.655 0.981 25.123 2.531 0.942
      0.15~0.18 0.127 167.976 0.870 59.312 4.326 0.923
      0.08~0.15 0.064 195.698 0.968 27.605 2.325 0.981
      下载: 导出CSV
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