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氨基改性SiO2气凝胶去除Cu(II)的性能与机制

翟红侠 赵越 李超凡 孔维丽 谢发之 李海斌

翟红侠, 赵越, 李超凡, 等. 氨基改性SiO2气凝胶去除Cu(II)的性能与机制[J]. 复合材料学报, 2023, 40(8): 4613-4624. doi: 10.13801/j.cnki.fhclxb.20221009.001
引用本文: 翟红侠, 赵越, 李超凡, 等. 氨基改性SiO2气凝胶去除Cu(II)的性能与机制[J]. 复合材料学报, 2023, 40(8): 4613-4624. doi: 10.13801/j.cnki.fhclxb.20221009.001
ZHAI Hongxia, ZHAO Yue, LI Chaofan, et al. Performance and mechanism of the amine-modified silica aerogel for the removal of Cu(II)[J]. Acta Materiae Compositae Sinica, 2023, 40(8): 4613-4624. doi: 10.13801/j.cnki.fhclxb.20221009.001
Citation: ZHAI Hongxia, ZHAO Yue, LI Chaofan, et al. Performance and mechanism of the amine-modified silica aerogel for the removal of Cu(II)[J]. Acta Materiae Compositae Sinica, 2023, 40(8): 4613-4624. doi: 10.13801/j.cnki.fhclxb.20221009.001

氨基改性SiO2气凝胶去除Cu(II)的性能与机制

doi: 10.13801/j.cnki.fhclxb.20221009.001
基金项目: 国家自然科学基金(52003003);安徽省矿山生态修复工程实验室开放课题(KS-2022-003);安徽省先进建筑材料国际联合研究中心基金(JZCL014 ZZ)
详细信息
    通讯作者:

    李海斌,硕士,讲师,研究方向为环境功能材料的制备及应用 E-mail: lihb@ahjzu.edu.cn

  • 中图分类号: TQ352;TB332

Performance and mechanism of the amine-modified silica aerogel for the removal of Cu(II)

Funds: National Natural Science Foundation of China (52003003); Opening Foundation of Anhui Province Engineering Laboratory for Mine Ecological Remediation (KS-2022-003); Fund Project of Anhui Province International Research Center on Advanced Building Materials (JZCL014 ZZ)
  • 摘要: 为有效去除液相中重金属Cu(II),以正硅酸乙酯为原料、3-氨丙基三乙氧基硅烷为氨基化试剂,通过共缩聚法合成氨基改性SiO2气凝胶(NG)。系统考察pH、离子强度、时间、温度等因素对NG去除Cu(II)的影响,结合吸附动力学模型、吸附等温模型、吸附热力学、位点能量分布理论分析其吸附机制。研究结果表明:pH在3.00~6.00条件下,Cu(II)吸附量随pH升高而增大。离子强度由0 mol/L增至0.08 mol/L时,Cu(II)吸附量受抑制作用呈逐渐降低趋势,FTIR分析显示NG与Cu(II)主要形成外层络合物。NG吸附Cu(II)时间在8 h内基本达到平衡,其吸附主要经过边界层扩散、颗粒内扩散与化学吸附等过程,且该吸附过程最符合准二级动力学模型与Freundlich模型。温度升高有利于促进吸附反应发生,Cu(II)最大吸附量达到130.45 mg/g,其吸附过程属吸热、熵增加的自发反应。位点能量分布显示随吸附反应进行,Cu(II)优先占据NG上高能量吸附位点,再占据低能量吸附位点,NG吸附Cu(II)的主要机制是外层络合与静电作用。

     

  • 图  1  氨基改性SiO2气凝胶(NG)的SEM图像和实物照 (a)、表面接触角 (b)、 XRD图谱 (c)、N2吸附-脱附等温线与孔径分布曲线 (d)

    Figure  1.  SEM and physical image of amine-modified silica aerogel (NG) (a), contact angle of the surface (b), XRD pattern (c), nitrogen absorption-desorption isotherms and pore size distribution (d)

    图  2  pH对NG吸附Cu(II)的影响(ρ0=20 mg/L, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (a)、水溶液中Cu(II)分布形态 (b)

    ρ0—Initial mass concentration; I—Ionic strength; T—Adsorption temperature; m—Quality of the NG; V—Volume of solution

    Figure  2.  Effect of pH on absorption of Cu(II) by NG (ρ0=20 mg/L, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (a), speciation of Cu(II) in the system (b)

    图  3  离子强度对NG吸附Cu(II)的影响(ρ0=20 mg/L, pH=5.15, T=298 K, m=0.02 g, V=50 mL) (a)、NG吸附Cu(II)前后FTIR图谱(ρ0=20 mg/L, pH=5.15, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (b)

    Figure  3.  Effect of ionic strength on absorption of Cu(II) by NG (ρ0=20 mg/L, pH=5.15, T=298 K, m=0.02 g, V=50 mL) (a), FTIR spectra of amine-modified silica aerogel before and after Cu(II) adsorption (ρ0=20 mg/L, pH=5.15, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (b)

    图  4  NG吸附Cu(II)的动力学曲线(ρ0=20 mg/L, pH=5.15, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (a)、颗粒内扩散模型拟合曲线(b)

    Figure  4.  Kinetic curves of Cu(II) adsorption by NG (ρ0=20 mg/L, pH=5.15, I=0 mol, T=298 K, m=0.02 g, V=50 mL) (a), Plot of intra-particle diffusion (b)

    图  5  不同等温模型对NG吸附Cu(II)的非线性拟合

    Figure  5.  Nonlinear fitting curves of Cu(II) absorption onto NG under different models

    图  6  NG吸附Cu(II)的表面溶质与溶剂之间吸附能量差(a)和位点能量分布(b)

    Figure  6.  Adsorption energy difference between surface solute and solvent on NG for Cu(II) (a) and site energy distribution (b)

    图  7  XPS全谱(a)、Cu2p精细谱(b)、N1s精细谱(c)、C1s精细谱(d)、O1s精细谱(e)、Si2p精细谱(f)

    Figure  7.  XPS survey spectrum (a), Cu2p fine spectrum (b), N1s fine spectrum (c), C1s fine spectrum (d), O1s fine spectrum (e), Si2p fine spectrum (f)

    图  8  NG去除Cu(II)机制

    Figure  8.  Schematic of adsorption mechanism of Cu(II) by the NG

    表  1  NG吸附Cu(II)的动力学模型参数

    Table  1.   Kinetic model parameters for Cu(II) adsorption onto NG

    Kinetic modelParameterResult
    Pseudo-first order modelqe,c/(mg·g−1)40.6704
    k1/(min−1)0.0217
    R20.9053
    Pseudo-second order modelqe,c/(mg·g−1)45.1501
    k2/(g·mg−1·min−1)0.0006
    R20.9653
    Intra-partical diffusion modelkp1, kp2/(mg·g−1·min−0.5)6.1698, 1.1281
    C1, C2−7.7112, 17.6597
    R12, R220.9760, 0.9538
    Notes: qe,c—Theoretical calculation of adsorption capacity; k1, k2 and kp—Rate constans for the pseudo-first order, pseudo-second order and intraparticle diffusion, respectively; R2—Coefficient of determination; C—Desorption constant.
    下载: 导出CSV

    表  2  不同温度下Cu(II)在NG上吸附的等温模型参数

    Table  2.   Isotherm parameters of Cu(II) adsorption onto NG at varying temperatures

    Model and parameter298 K308 K318 K
    Langmuir nonlinear fit${q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{7.39{\rho _{\text{e}}}}}{{1 + 0.05533{\rho _{\text{e}}}}}$$ {q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{14.15{\rho _{\text{e}}}}}{{1 + 0.10868{\rho _{\text{e}}}}} $${q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{16.43{\rho _{\text{e}}}}}{{1 + 0.11819{\rho _{\text{e}}}}}$
    R20.99130.99660.9958
    Freundlich nonlinear fit${q_{{\text{e}},{\text{c}}}}{\text{ = 29}}{\text{.55}}\rho _{\text{e}}^{0.2986}$${q_{{\text{e}},{\text{c}}}}{\text{ = 47}}{\text{.55}}\rho _{\text{e}}^{0.2080}$${q_{{\text{e}},{\text{c}}}}{\text{ = 54}}{\text{.45}}\rho _{\text{e}}^{0.1942}$
    R20.99800.99950.9997
    Sips nonlinear fit${q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{29.55{\rho _{\text{e}}}^{0.2987}}}{{1 + 0.00004{\rho _{\text{e}}}^{0.2987}}}$${q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{49.26{\rho _{\text{e}}}^{0.2525}}}{{1 + 0.08598{\rho _{\text{e}}}^{0.2525}}}$${q_{{\text{e}},{\text{c}}}}{\text{ = }}\dfrac{{54.45{\rho _{\text{e}}}^{0.1942}}}{{1 + 0.00006{\rho _{\text{e}}}^{0.1942}}}$
    R20.99760.99940.9996
    Temkin nonlinear fit${q_{{\text{e}},{\text{c}}}}{\text{ = }} - 3.86 + 25.67\ln {\rho _{\text{e}}}$${q_{{\text{e}},{\text{c}}}}{\text{ = 27}}{\text{.97}} + 20.49\ln {\rho _{\text{e}}}$${q_{{\text{e}},{\text{c}}}}{\text{ = }}35.97 + 20.74\ln {\rho _{\text{e}}}$
    R20.99520.99920.9990
    下载: 导出CSV

    表  3  不同种类气凝胶对Cu(II)吸附效果

    Table  3.   Cu(II) adsorption by different aerogels

    NumberSorbentReaction conditionAdsorption capacity/(mg·g-1)Reference
    1 Carbon aerogel pH=7.00, T=298 K, t=10 min 86.27 [30]
    2 MnFe2O4-cellulose aerogel pH=6.00, T=298 K, t=100 min 63.30 [31]
    3 Graphene oxide aerogel pH=6.30, T=313 K, t=30 min 29.59 [32]
    4 Porous alginate aerogel bead pH=4.50, T=298 K, t=950 min 126.82 [33]
    5 Graphene oxide/carboxymethyl chitosan aerogel pH=5.00, T=303 K, t=600 min 95.37 [34]
    6 Amine-modified sillica aerogel pH=5.00, T=318 K, t=720 min 130.45 Present study
    下载: 导出CSV

    表  4  NG吸附Cu(II)的热力学参数

    Table  4.   Thermodynamic parameters for the adsorption of Cu(II) onto NG

    T/KKCΔG/(kJ·mol−1)ΔH/(kJ·mol−1)ΔS/(J·(mol·K)−1)
    29829550−25.5024.21167.27
    30847550−27.58
    31854450−28.83
    Notes: T—Temperature; ΔG—Gibbs free energy; ΔH—Change in enthalpy during adsorption; ΔS—Adsorption process entropy change; KC—Modified constant.
    下载: 导出CSV
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出版历程
  • 收稿日期:  2022-08-11
  • 修回日期:  2022-09-05
  • 录用日期:  2022-09-17
  • 网络出版日期:  2022-10-09
  • 刊出日期:  2023-08-15

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