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聚乙烯亚胺交联膨润土对水中Cr(Ⅵ)的吸附性能与机制

孙志勇 张宇辰 吴喜军

孙志勇, 张宇辰, 吴喜军. 聚乙烯亚胺交联膨润土对水中Cr(Ⅵ)的吸附性能与机制[J]. 复合材料学报, 2024, 42(0): 1-12.
引用本文: 孙志勇, 张宇辰, 吴喜军. 聚乙烯亚胺交联膨润土对水中Cr(Ⅵ)的吸附性能与机制[J]. 复合材料学报, 2024, 42(0): 1-12.
SUN Zhiyong, ZHANG Yuchen, WU Xijun. Adsorption performance and mechanism of polyethyleneimine cross-linked bentonite for Cr (VI) in aqueous solution[J]. Acta Materiae Compositae Sinica.
Citation: SUN Zhiyong, ZHANG Yuchen, WU Xijun. Adsorption performance and mechanism of polyethyleneimine cross-linked bentonite for Cr (VI) in aqueous solution[J]. Acta Materiae Compositae Sinica.

聚乙烯亚胺交联膨润土对水中Cr(Ⅵ)的吸附性能与机制

基金项目: 国家自然科学基金资助项目(52064048);陕西省科技创新团队(2022TD-08)
详细信息
    通讯作者:

    孙志勇,硕士,教授,硕士生导师,研究方向为功能材料、环境污染治理技术 E-mail:sunzy11@126.com

  • 中图分类号: X703

Adsorption performance and mechanism of polyethyleneimine cross-linked bentonite for Cr (VI) in aqueous solution

Funds: National Natural Science Foundation of China (52064048); Shaanxi Provincial Science and Technology Innovation Team (2022TD-08)
  • 摘要: 为提高膨润土的吸附容量,通过交联反应将聚乙烯亚胺(PEI)引入3-氨丙基三乙氧基硅烷(APTES)改性膨润土(APTES/Bent)表面制备得到PEI交联膨润土(PEI-APTES/Bent-4),并采用FTIR、XRD和SEM等手段对其进行表征分析。以水中Cr(Ⅵ)为吸附对象,考察了PEI-APTES/Bent-4的吸附性能,探究了吸附机制和回收利用性。结果表明:PEI成功接枝于膨润土表面,其丰富的活性基团极大的促进了六价铬的去除。吸附最佳pH为2,随pH值增加吸附量降低。PEI-APTES/Bent-4对Cr(Ⅵ)的吸附符合Langmuir等温模型和拟二级动力学模型,吸附过程为化学吸附和单层吸附,在313 K时最大理论吸附量达137.50 mg·g−1。热力学研究表明该吸附为自发吸热过程。结合吸附实验、FTIR和XPS分析推测得出PEI-APTES/Bent-4对Cr(Ⅵ)的吸附机制主要为静电作用、还原和螯合。经6次循环后吸附剂仍保持较好的吸附性能。PEI-APTES/Bent-4去除水中Cr(Ⅵ)具有较大的应用前景。

     

  • 图  1  聚乙烯亚胺交联膨润土(PEI-APTES/Bent)的制备过程

    Figure  1.  Preparation process of polyethyleneimine cross-linked bentonite (PEI-APTES/Bent)

    图  2  Bent、APTES/Bent和PEI-APTES/Bent-4的FTIR图谱(a)、XRD图谱(b)和TGA曲线(c)

    Figure  2.  FTIR spectra(a), XRD pattern(b) and TGA curves (c) of Bent, APTES/Bent and PEI-APTES/Bent-4

    图  3  Ben、APTES/Bent和PEI-APTES/Bent-4的SEM-EDS图像

    Figure  3.  SEM-EDS images of Ben, APTES/Bent, PEI-APTES/Bent-4

    图  4  不同样品对Cr(Ⅵ)的吸附量

    Figure  4.  The adsorption capacity of different samples for Cr(Ⅵ)

    图  5  pH对吸附Cr(Ⅵ)的影响(a)与PEI-APTES/Bent-4的Zeta电位曲线(b)

    Figure  5.  Effect of pH on the adsorption of Cr (VI) (a) and the Zeta potential curves of Bent and PEI-APTES/Bent-4(b)

    图  6  吸附时间对Cr(Ⅵ)吸附量的影响(a)与动力学模型拟合:(b)准一级动力学模型拟合;(c)准二级动力学模型拟合

    Figure  6.  Effect of adsorption time on the adsorption capacity of Cr (Ⅵ)(a) and kinetics model fitting: (b)Pseudo-first-order kinetic model; (c) pseudo-second-order kinetic model

    图  7  PEI-APTES/Bent-4吸附Cr(Ⅵ)等温吸附模型拟合

    Figure  7.  Isothermal adsorption model fitting of Cr (Ⅵ) adsorption by PEI-APTES/Bent-4

    图  8  PEI-APTES/Bent-4吸附Cr(Ⅵ)前后的红外光谱图

    Figure  8.  FTIR spectra of PEI-APTES/Bent-4 before and after adsorption of Cr (Ⅵ)

    图  9  PEI-APTES/Bent-4吸附Cr(Ⅵ)前后的XPS图谱:全图谱(a);Cr 2 p图谱(b)

    Figure  9.  XPS spectra of PEI-APTES/Bent-4 before and after adsorption of Cr(Ⅵ): full spectrum (a), Cr 2 p spectrum (b)

    图  10  PEI-APTES/Bent-4吸附Cr(Ⅵ)的机制

    Figure  10.  Mechanism diagram of PEI-APTES/Bent-4 adsorption of Cr (Ⅵ)

    图  11  循环次数对PEI-APTES/Bent-4吸附Cr((Ⅵ)的影响

    Figure  11.  The Effect of Cycle Times on the Adsorption of Cr (Ⅵ) by PEI-APTES/Bent-4

    表  1  PEI-APTES/Bent-4与其他改性膨润土的Cr(VI)吸附量比较

    Adsorbentqm/mg·g-1Ref.
    CTMAB/Bent27.472[37]
    AC-Fe3O4/Bent29.32[38]
    Citric acid/MBent16.67[39]
    polyacrylic acid-Al/Bent3.125[40]
    Fe3O4-PDA-SDBS/Bent103.6[41]
    Chitosan-NaOH/Bent2.72[42]
    Cetylpyridinium chloride/Bent46.03[43]
    Chitosan/Bent16.40[44]
    PEI-APTES/Bent-4137.50This study
    Notes: CTMAB—Cetyltrimethylammonium bromide; MBent—Magnetic Bentonite; AC—Activated Carbon; PDA—Polydopamine; SDBS—Sodium dodecyl benzene sulfonate.
    下载: 导出CSV

    表  1  PEI-APTES/Bent-4对Cr(Ⅵ)的吸附动力学参数

    Table  1.   Kinetic model fitting parameters for Cr(Ⅵ) adsorption on PEI-APTES/Bent-4

    adsorbent Pseudo-first-order Pseudo-second-order
    qe/(mg·g−1) K1/min−1 R2 qe/(mg·g−1) K2/(g·mg−1·min−1) R2
    PEI-APTES/Bent-4 78.39 0.1286 0.9898 131.06 0.0076 0.9997
    Notes: qe—Amount of adsorption at equilibrium; K1—Quasi-first-order kinetic model constant; K2—Quasi-second-order kinetic model constant; R—Correlation coefficient.
    下载: 导出CSV

    表  2  Langmuir和Freundlich模型参数

    Table  2.   Langmuir and Freundlich model parameters

    T/K Langmuir Freundlich
    qm/(mg·g−1) KL/(L·mg−1) RL R2 KF/(mg1-(1/n)·L1/n·g−1) n R2
    293 132.02 0.4046 0.0049-0.1099 0.9869 58.98 6.475 0.8479
    303 135.68 0.6558 0.0030-0.0708 0.9627 65.12 6.893 0.8711
    313 137.50 1.2208 0.0016-0.03935 0.9565 71.11 7.468 0.8835
    Notes: qm−Maximum adsorption capacity; KL−Adsorption equilibrium constant of Langmuir model; KF−Adsorption equilibrium constant of Freundlich model; n−Adsorption strength constant in the Freundlich model; RL−Separation constant; R2−linear correlation coefficient.
    下载: 导出CSV

    表  3  PEI-APTES/Bent-4与其他改性膨润土Cr(VI)吸附量比较

    Table  3.   Comparison of Cr (VI) adsorption capacity between PEI-APTES/Bent-4 and other modified bentonite

    Adsorbent Maximum adsorption capacity/(mg·g−1) Ref.
    CTMAB/Bent 27.472 [37]
    AC- Fe3O4/Bent 29.32 [38]
    Citric acid/MBent 16.67 [39]
    polyacrylic acid-Al/Bent 3.125 [40]
    Fe3O4-PDA-SDBS/Bent 103.6 [41]
    Chitosan-NaOH/Bent 2.72 [42]
    Cetylpyridinium chloride/Bent 46.03 [43]
    Chitosan/Bent 16.40 [44]
    PEI-APTES/Bent-4 137.50 This study
    Notes:CTMAB—Cetyltrimethylammonium bromide; AC—Activated Carbon; PDA—Polydopamine; MBent—Magnetic Bentonite; SDBS—Sodium dodecyl benzene sulfonate.
    下载: 导出CSV

    表  4  吸附Cr(Ⅵ)的热力学参数

    Table  4.   Thermodynamic parameters for adsorption of Cr(Ⅵ)

    T/K ΔG0/(kJ·mol−1) ΔH0/(kJ·mol−1) ΔS0/(J·mol−1)
    293 −6.511
    303 −7.439 23.73 103.11
    313 −8.578
    Notes: ∆G0—Gibbs free energy change; ∆H0—Enthalpy change; ∆S0—Entropy change.
    下载: 导出CSV
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出版历程
  • 收稿日期:  2024-03-18
  • 修回日期:  2024-04-15
  • 录用日期:  2024-04-15
  • 网络出版日期:  2024-05-23

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