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Preparation of a N, S, P co-doped and oxidized porous carbon for the efficient adsorption of uranium(VI)

LIU Yan LIU Xiao-peng DAI Ying WANG Yun YUAN Ding-zhong LIU Jin-biao CHEW Jia-wei

刘妍, 刘晓鹏, 戴荧, 王云, 袁定重, 刘晋彪, ChewJia-wei. 杂原子掺杂的羧酸功能化炭材料的制备及其吸附U(VI)性能. 新型炭材料, 2021, 36(6): 1138-1148. doi: 10.1016/S1872-5805(21)60055-0
引用本文: 刘妍, 刘晓鹏, 戴荧, 王云, 袁定重, 刘晋彪, ChewJia-wei. 杂原子掺杂的羧酸功能化炭材料的制备及其吸附U(VI)性能. 新型炭材料, 2021, 36(6): 1138-1148. doi: 10.1016/S1872-5805(21)60055-0
LIU Yan, LIU Xiao-peng, DAI Ying, WANG Yun, YUAN Ding-zhong, LIU Jin-biao, CHEW Jia-wei. Preparation of a N, S, P co-doped and oxidized porous carbon for the efficient adsorption of uranium(VI). New Carbon Mater., 2021, 36(6): 1138-1148. doi: 10.1016/S1872-5805(21)60055-0
Citation: LIU Yan, LIU Xiao-peng, DAI Ying, WANG Yun, YUAN Ding-zhong, LIU Jin-biao, CHEW Jia-wei. Preparation of a N, S, P co-doped and oxidized porous carbon for the efficient adsorption of uranium(VI). New Carbon Mater., 2021, 36(6): 1138-1148. doi: 10.1016/S1872-5805(21)60055-0

杂原子掺杂的羧酸功能化炭材料的制备及其吸附U(VI)性能

doi: 10.1016/S1872-5805(21)60055-0
基金项目: 国家自然科学基金项目(22166001,21966005, 22066002),江西省自然科学基金项目(20202BABL2030012,20192BAB202007,20192ACB21001),东华理工大学核资源与环境国家重点实验室开放基金(NRE1926),省级大学生创新创业训练计划项目(S202110405019)
详细信息
    通讯作者:

    刘 妍,副教授. E-mail:fzliuyan1986@163.com

    CHEW Jia-wei,副教授. E-mail:JChew@ntu.edu.sg

  • 中图分类号: TQ127.1+1

Preparation of a N, S, P co-doped and oxidized porous carbon for the efficient adsorption of uranium(VI)

Funds: We appreciate the financial support from the National Natural Science Foundation of China (No.22166001, 21966005, 22066002 ), the Jiangxi Provincial Natural Science Foundation (No.20202BABL203001, 20192BAB202007, 20192ACB21001), the Opening fund project of State Key Laboratory of Nuclear Resources and Environment, East China University of Technology (NRE1926), Provincial College Students' Innovation and Entrepreneurship Training Program (S202110405019)
More Information
  • 摘要: 通过煅烧前驱体聚磷腈,制备了掺杂N,P和O的羧基官能化炭材料(CS―COOH)。利用TEM,SEM,XPS和FTIR技术确定了CS―COOH结构。研究了CS―COOH从水溶液中吸附U(VI)情况,结果表明,吸附动力学符合准二级动力学模型,通过Langmuir模型计算得到在298 K下材料的最大吸附量为402.9 mg/g。CS―COOH在5次吸附-解吸循环后表现出良好的吸附结果。根据XPS分析,材料较好的U(VI)吸附能力主要归因于羧基及杂原子与铀酰离子之间的强共价键结合。
  • FIG. 1081.  FIG. 1081.

    FIG. 1081.. 

    Figure  1.  Preparation process of CS-COOH.

    Figure  2.  SEM, TEM and HRTEM images of (a, c) CS and (b, d-f) CS-COOH.

    Figure  3.  N2 adsorption-desorption isotherms of CS and CS―COOH.

    Figure  4.  (a) FTIR spectra of CS and CS―COOH and (b) high resolution XPS spectrum of CS―COOH.

    Figure  5.  (a) Effect of initial solution pH on the adsorption of U(VI) by CS and CS―COOH. (T = 298 K, m = 5 mg, C0 = 50 mg L−1 and V = 30 mL); (b) Distribution of U(VI) species in aqueous solutions with a total concentration of 50 mg L−1 and pH values ranging from 1 to 12 (calculated by using a Medusa program).

    Figure  6.  (a) Effect of (a) the contact time (C0 = 50 mg L-1) and (b) the initial concentration on the adsorption of U(VI) by CS and CS-COOH. (T = 298 K, m = 5 mg, V = 30 mL and pH = 6)

    Figure  7.  (a) Pseudo-first-order and (b) pseudo-second-order adsorption kinetics models of U(VI) adsorption by CS and CS―COOH.

    Figure  8.  (a) Langmuir and (b) Freundlich isotherms of U(VI) adsorbed by CS and CS-COOH.

    Figure  9.  (a) Effect of the temperature on the equilibrium adsorption capacities of U(VI) on CA and CS―COOH (m = 5 mg, V = 30 mL, C0 = 50 mg L−1, t=180 min and pH = 6) and (b) the equilibrium constants as a function of 1/T of U(VI) adsorption by CS and CS―COOH.

    Figure  10.  (a) Selective adsorption capacity in presence of coexistent ions (C0 = 0.5 mmol L−1) and (b) adsorption performance of U(VI) by CS―COOH over 5 cycles (C0 = 50 mg L−1). (m = 5 mg, V = 30 mL, T = 298 K and pH = 6).

    Figure  11.  (a) XPS survey spectrum of CS-COOH-U and the high resolution XPS spectra of (b) C1s, (c) O1s, (d) N1s, (e) P2p and (f) S2p.

    Figure  12.  FTIR spectra of CS-COOH and CS-COOH-U.

    Table  1.   Kinetic parameters for adsorption of U(VI) by CS and CS-COOH.

    Materialsqe,exp (mg g−1)Pseudo-first-order modelPseudo-second-order model
    q1,cal (mg g−1)k1 (/min)R2q2,cal (mg g−1)k2 (g mg−1·min−1)R2
    CS150.3498.698.21×10−30.905173.312.88×10−40.9764
    CS-COOH238.20190.493.34×10−20.939250.431.85×10−40.9957
    下载: 导出CSV

    Table  2.   Parameters of Langmuir and Freundlich isotherm models for adsorption of U(VI) by CS and CS-COOH.

    MaterialsLangmuir isothermFreundlich isotherm
    KLqm (mg g−1)R2KFnR2
    CS7.80229.360.99764.05×10−30.310.9423
    CS-COOH0.018402.900.922712.661.400.9033
    下载: 导出CSV

    Table  3.   The thermodynamic parameters for U(VI) adsorption by CS and CS-COOH.

    MaterialsΔH
    (kJ mol−1)
    ΔS
    (J mol−1 K−1)
    ΔG (kJ mol−1)
    288
    (K)
    298
    (K)
    303
    (K)
    313
    (K)
    318
    (K)
    CS49.82216.16−12.41−14.57−15.65−17.81−18.89
    CS−COOH7.7391.89−18.74−19.66−20.12−21.04−21.50
    下载: 导出CSV
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出版历程
  • 收稿日期:  2020-02-26
  • 修回日期:  2020-12-10
  • 网络出版日期:  2021-03-25
  • 刊出日期:  2021-12-01

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