Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration

doi:10.1007/s11705-023-2358-0

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (12) : 2037-2049 https://doi.org/10.1007/s11705-023-2358-0

RESEARCH ARTICLE

Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration

Jiafeng Ouyang^1,², Wenlu Guo^2,³, Lin Wang², Changming Nie³, Dadong Shao¹(

), Weiqun Shi², Liyong Yuan²(

)

¹. School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
². Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
³. School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China

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Abstract

Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years, it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic particles. Herein, we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide. The prepared materials exhibited excellent properties for U(VI) ions removal from aqueous solutions under various conditions. The experimental data show that the U(VI) adsorption features fast adsorption kinetics, high adsorption capacity and ideal selectivity toward U(VI). The adsorption process is of spontaneous and endothermic nature and ionic strength independence, and the adsorbents can be easily regenerated by acid treatment. Compared to pristine KIT-6, the introduction of magnetism does not reduce the efficiency of the material to remove U(VI) while exerting its role as a recovery adsorbent. The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.

Keywords magnetic nanoparticle 3D mesoporous silica amino functionalization adsorption of U(VI) acid resistance

Corresponding Author(s): Dadong Shao,Liyong Yuan

Online First Date: 18 October 2023 Issue Date: 30 November 2023

Cite this article:

Jiafeng Ouyang,Wenlu Guo,Lin Wang, et al. Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration[J]. Front. Chem. Sci. Eng., 2023, 17(12): 2037-2049.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2358-0
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I12/2037

Scheme1 Schematic diagram of preparation of MKIT-6-XN.

Fig.1 SEM images of (a) Fe₃O₄, (b) MKIT-6, and (c) MKIT-6-40N; TEM images of (d) KIT-6, (e) MKIT-6, and (f) MKIT-6-40N.

Fig.2 Characterization of magnetic KIT-6 nanocomposite and its amino derivatives. (a) Wide-angle PXRD patterns of Fe₃O₄ and MKIT-6; (b) small-angle PXRD patterns of KIT-6, MKIT-6 and MKIT-6-40N; (c) FTIR spectra of KIT-6, MKIT-6, MKIT-6-40N, U(VI) loaded MKIT-6-40N; (d) TGA profile of MKIT-6 and MKIT-6-40N; (e) N₂ adsorption/desorption isotherm of KIT-6, MKIT-6 and MKIT-6-40; (f) the respective non-local density functional theory PSDs calculated from the desorption branch.

Tab.1 N₂ adsorption results

Fig.3 (a) Effect of pH on the U(VI) adsorption (m_adsorbent/V_solution = 0.4 mg·mL^–1, [U]_initial = 100 mg·L^–1, T = 288 K); (b) zeta potentials of KIT-6, MKIT-6 and MKIT-6-40N as a function of pH.

Fig.4 The adsorption kinetics study of KIT-6, MKIT-6 and MKIT-6-40N. (a) Effect of the contacting time (pH = 5.0, m_adsorbent/V_solution = 0.4 mg·mL^–1, [U]_initial = 100 mg·L^–1, T = 288 K); (b) the scattered points represent experiment data of MKIT-6-40N, while the red lines represent fitting by the pseudo-second-order model and the black dotted lines represent fitting by the pseudo-first-order model.

Tab.2 Kinetics model constants and correlation coefficients for U(VI) adsorption

Tab.3 Isotherm model constants and correlation coefficients for U(VI) adsorption

Fig.5 Adsorption isotherms study to MKIT-6-40N (pH = 5.0, m_adsorbent/V_solution = 0.4 mg·mL^–1, [U]_initial = 100 mg·L^–1, T = 288 K; the scattered points represent experimental data, while the red solid line represents the fitting by Langmuir model).

Fig.6 (a) Adsorption capacity of MKIT-6-40N for U(VI) at different temperatures, pH = 5.0, m_adsorbent/V_solution = 0.4 mg·mL^–1, [U]_initial = 100 mg·L^–1; (b) relationship curve between lnK_d and T^–1.

Tab.4 Thermodynamic parameters for the U(VI) adsorption

Fig.7 Impact of ionic strength on the U(VI) ion removal (pH = 5.0, [U]_initial = 100 mg·L^–1, m_adsorbent/V_solution = 0.4 mg·mL^–1, T = 288 K).

Fig.8 Competitive adsorption in the removal of U(VI) ions (pH = 5.0, [U]_initial = 100 mg·L^–1, m_adsorbent/V_solution = 0.4 mg·mL^–1, T = 288 K).

Fig.9 The image of magnetic separation.

Fig.10 (a) Released Fe in HNO₃ solutions and (b) the changes of adsorption capacity in 4 cycles, pH = 5.0, [U]_initial = 100 mg·L^–1, m_adsorbent/V_solution = 0.4 mg·mL^–1, T = 288 K.

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