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木质素表面功能化MXene纳米片的制备及其对U(VI)的吸附性能

李仕友 乔记帅 杨宇彪 熊芷毓 王国华

李仕友, 乔记帅, 杨宇彪, 等. 木质素表面功能化MXene纳米片的制备及其对U(VI)的吸附性能[J]. 复合材料学报, 2024, 42(0): 1-15.
引用本文: 李仕友, 乔记帅, 杨宇彪, 等. 木质素表面功能化MXene纳米片的制备及其对U(VI)的吸附性能[J]. 复合材料学报, 2024, 42(0): 1-15.
Li Shiyou, Qiao Jishuai, Yang Yubiao, et al. Preparation of lignin surface-functionalized MXene nanosheets and its U(VI)adsorption properties[J]. Acta Materiae Compositae Sinica.
Citation: Li Shiyou, Qiao Jishuai, Yang Yubiao, et al. Preparation of lignin surface-functionalized MXene nanosheets and its U(VI)adsorption properties[J]. Acta Materiae Compositae Sinica.

木质素表面功能化MXene纳米片的制备及其对U(VI)的吸附性能

基金项目: 湖南省自然科学基金项目(2022JJ30490);国家自然科学基金项目(51904155)
详细信息
    通讯作者:

    王国华,博士,副教授,硕士生导师,研究方向为放射性污染治理与资源化 E-mail: wghcsu@163.com

  • 中图分类号: TB333

Preparation of lignin surface-functionalized MXene nanosheets and its U(VI)adsorption properties

Funds: The Natural Science Foundation of Hunan Province (2022JJ30490); The National Natural Science Foundation of China(51904155)
  • 摘要: 为了进一步改善MXene纳米材料对模拟放射性废水中U(Ⅵ)的吸附性能,利用天然资源酶水解木质素(EHL)作为生物表面活性剂对MXene进行表面功能化处理,采用SEM-EDS、XRD及FTIR对改性前后的材料进行了表征分析,并在吸附实验中探究了pH、温度、反应时间、干扰离子及不同初始U(Ⅵ)浓度等因素对除U(Ⅵ)效果的影响。结果表明,EHL阻止了MXene纳米片的聚集堆叠,并且引入了大量活性官能团,提高了EHL功能化MXene纳米片的吸附性能。在MXene与EHL的质量比为1∶5、投加量为0.1 g·L−1、pH为5、温度为303 K时,对U(VI)的最大吸附容量为231.95 mg·g−1。此外,吸附动力学和等温线分析表明,拟二阶动力学模型和Frendlich等温线模型能很好的拟合此吸附过程,热力学分析表明其吸附过程是自发吸热的。经历5次循环再生后,对U(VI)的去除率仍在80%以上。表征分析结果表明,MX/EHL与U(VI)之间相互作用机制包括离子交换、静电吸引以及与含氧官能团之间的络合作用。基于此研究,MX/EHL作为一种环境友好型吸附材料,对去除废水中的U(VI)具有巨大潜力。

     

  • 图  1  Ti3C2Tx(MX)/酶水解木质素(EHL)的主要制备步骤

    Figure  1.  The main preparation processes of Ti3C2Tx (MX)/ enzymatically hydrolyzed lignin (EHL)

    图  2  MX(a、b)和MX/EHL(c、d)的SEM图;MX(e)和MX/EHL(f)的EDS能谱

    Figure  2.  SEM images of MX(a、b) and MX/EHL(c、d);EDS patterns of MX(e) and MX/EHL(f)

    图  3  MAX(Ti3AlC2)、MX和MX/EHL的XRD光谱(a);MX和MX/EHL的N2吸脱附及孔径图(b)

    Figure  3.  XRD spectra of MAX(Ti3AlC2)、MX and MX/EHL(a); N2 adsorption-desorption and pore size of MX and MX/EHL (b)

    图  4  MX、EHL和MX/EHL吸附前后的FTIR图谱

    Figure  4.  FTIR spectra of MX、EHL and MX/EHL before and after adsorption

    图  5  不同配比MX/EHL吸附剂对U(VI) 的吸附效率对比

    Figure  5.  Comparison of adsorption efficiency of different ratios of MX/EHL adsorbents on U(VI)

    图  6  不同MX/EHL投加量对吸附U(VI) 的影响

    Figure  6.  Effect of different MX/EHL dosage on adsorption of U(VI)

    图  7  (a)不同pH值下U(VI) 的形态分布曲线图;(b)不同pH值对MX/EHL吸附U(VI)性能的影响

    Figure  7.  (a) Morphological distribution curves of U(VI) at different pH values; (b) Effect of different pH values on the adsorption performance of U(VI) by MX/EHL

    图  8  (a)接触时间对MX/EHL吸附U(VI)的影响;(b)拟一级动力学;(c)拟二级动力学;(d)颗粒内扩散模型

    Figure  8.  (a) Effect of contact time on U(VI) adsorption by MX/EHL; (b) Pseudo-first-order; (c) Pseudo-second-order; (d) Intraparticle diffusion model

    图  9  MX/EHL吸附U(VI)的Langmuir(a)、Freundlich(b)和Dubinin-Radushkevich(c)等温吸附模型拟合曲线;(d)lnK0与1/T的线性拟合

    Figure  9.  Fitting curve of Langmuir(a)、 Freundlich (b) and Dubinin‒Radushkevich (c) isothermal adsorption model of U(VI) adsorption by MX/EHL; (d) Linear fit of lnK0 versus 1/T

    图  10  不同种类竞争离子对MX/EHL吸附U(VI)的影响

    Figure  10.  effect of different competitive ions on adsorption of U(VI) on MX/EHL

    图  11  MX/EHL吸附剂循环再生试验

    Figure  11.  MX/EHL adsorbent cycle regeneration experiment

    图  12  (a)吸附前后MX/EHL全谱图;(b)U 4 f光谱图;(c、d)O 1 s光谱图;(e、f)C 1 s光谱图;

    Figure  12.  (a)full spectrum of MX/EHL before and after adsorption; (b) U 4 f spectrum; (c、d) O 1 s spectrum; (e、f) C 1 s spectrum

    表  1  MX和MX/EHL的孔隙结构参数

    Table  1.   Pore structure parameters of MX and MX/EHL

    MaterialSurface area/
    (m2·g−1)
    Pore volume/
    (cm3·g−1)
    Pore diameter/
    nm
    MX3.82970.010010.4628
    MX/EHL8.77510.045520.7320
    下载: 导出CSV

    表  2  MX/EHL对U(VI)的吸附动力学参数

    Table  2.   The adsorption kinetic parameters of U(VI) on MX/EHL

    Kinetic model Name of sample MX MX/EHL(1∶4) MX/EHL(1∶5)
    qe,exp/(mg·g−1) 35.22 46.92 48.24
    Pseudo-first-order k1/min−1 0.017 0.017 0.018
    qe,cal/(mg·g−1) 3.487 2.737 2.502
    R2 0.882 0.949 0.930
    Pseudo-second-order k2/min−1 0.021 0.027 0.030
    qe,cal/(mg·g−1) 35.51 47.13 48.43
    R2 0.999 0.999 0.999
    Intraparticle diffusion kp1/(mg·(g·min0.5)−1) 0.688 0.282 0.338
    C1 29.782 43.819 45.002
    R12 0.973 0.958 0.981
    Intraparticle diffusion kp2/(mg·(g·min0.5)−1) 0.406 0.324 0.303
    C2 31.266 43.568 45.243
    R22 0.989 0.986 0.994
    kp3/(mg·(g·min0.5)−1) 0.015 0.058 0.035
    C3 35.029 46.175 47.794
    R32 0.804 0.653 0.615
    Notes: qe,exp is the actual adsorption capacity at adsorption equilibrium; qe,cal is the calculated adsorption capacity at adsorption equilibrium; k1 and k2 are the adsorption rate constants of the pseudo-first and pseudo-second, respectively ; R2 is the correlation coefficient; kp1, kp2, kp3 are the adsorption rate constants of intraparticle diffusion.
    下载: 导出CSV

    表  3  Langmuir、Freundlich和Dubinin‒Radushkevich吸附等温线模型的相关参数

    Table  3.   Parameters associated with Langmuir, Freundlich and Dubinin-Radushkevich adsorption isotherm models

    T/K Langmuir Freundlich Dubinin‒Radushkevich
    qmax/(mg·g−1) KL/(L∙mg−1) R2 KF 1/n R2 qDR E R2
    293 K 205.493 0.164 0.890 48.175 0.399 0.982 115.99 1.879 0.554
    298 K 217.057 0.221 0.925 58.802 0.378 0.989 129.09 2.077 0.607
    303 K 231.947 0.251 0.924 65.565 0.379 0.997 138.33 2.337 0.627
    Notes: qmax is the maximum adsorption capacity; KL is the Langmuir adsorption equilibrium constant; KF and n are the constants that are related to the adsorption capacity and the adsorption intensity, respectively; R is the universal gas constant (8.312 J·mol−1·K−1), T is the temperature (K); E is the average free energy of adsorption.
    下载: 导出CSV

    表  5  不同吸附剂对U(VI)的吸附去除效果对比

    Table  5.   Comparison of adsorption and removal effects of different adsorbents on U(VI)

    Adsorbent pH T/K qmax/(mg·g−1) Reference
    C-TC 5 308 165.43 [20]
    MXene/SA 4 298 126.82 [34]
    C-TC-CS 6 313 141.96 [36]
    PANI/Ti3C2Tx 5 298 102.8 [37]
    PAO/Ti3C2Tx 4 298 98.04 [38]
    Ti3C2-AO-PA 8.3 298 81.1 [47]
    MX/EHL 5 303 231.95 This work
    Notes: C-TC is Chloroacetic acid modified-Ti3C2Tx; MXene/SA is MXene composite sodium alginate gel microsphere; C-TC-CS is chloroacetic acid-modified MXene-CS gel microspheres; PANI/Ti3C2Tx is polyaniline modified Mxene composites; PAO/Ti3C2Tx is Polyamidoxime functionalized MXene composite; Ti3C2-AO-PA is polyamide enhanced amidoxime-functionalized Ti3C2 nanosheet; T is the reaction temperature; qmax is the maximum adsorption capacity.
    下载: 导出CSV

    表  4  MX/EHL吸附U(VI)的热力学参数

    Table  4.   Thermodynamic parameters of MX/EHL adsorption of U(VI)

    T/K lnK0 ΔG0/(kJ·mol−1) ΔH0/(kJ·mol−1) ΔS0/(J·(mol·K)−1)
    293 K 4.69 −11.43 38.89 175.26
    298 K 5.00 −12.39
    303 K 5.23 −13.18
    Notes: T is the thermodynamic temperature; K0 is the equilibrium constant at different temperatures; ΔH0 is the standard enthalpy change; ΔG0 is the standard free energy change; ΔS0 is the standard entropy change.
    下载: 导出CSV
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  • 收稿日期:  2023-11-16
  • 修回日期:  2023-12-20
  • 录用日期:  2023-12-23
  • 网络出版日期:  2024-01-18

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