Experiment on Influence of Flow Velocity and Medium Particle Size on As(Ⅲ) Migration
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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.Abstract: To understand the influence of groundwater velocity and medium particles on As(Ⅲ) migration in the riparian zone, natural river sand is selected as the medium, and groundwater solutions containing As(Ⅲ) as commonly seen in some riparian zones are prepared to carry out batch experiments and dynamic column experiments. Combing with the characterization analysis, the influence and mechanism of velocity and medium particle size on As(Ⅲ) migration are discussed. The results show follows: (1) The adsorption equilibrium time of As(Ⅲ) is longer for the smaller particle size of river sand. The equilibrium adsorption capacity (Qe) of As (Ⅲ) on the river sand decreases with the increase of its particle sizes (except for river sand with a particle size of 0.15-0.18 mm), and the maximum amount (Qm) of monolayer adsorption shows a decreasing trend with the increase of particle size. (2) As(Ⅲ) migration in the column filled with river sand is significantly affected by the particle size and velocity. On one hand, the river sand of the smaller particle size has a larger specific surface area, which usually leads to longer interaction time between aqueous solutions and solid medium, thus limiting the groundwater flushing rate. This is not conducive to the migration of As(Ⅲ) in river sand. On the other hand, the higher flowing velocity leads to a stronger hydraulic shear force in the void channel. Meanwhile, the increase of turbulence intensity reduces the thickness of the retained boundary layer, which is conducive to the migration of As(Ⅲ) in river sand.
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Key words:
- flow rate /
- particle size /
- As(Ⅲ) /
- migration /
- hydrogeology
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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 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 
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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
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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 Qt=βIn(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)
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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
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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
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