A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications for the ‘‘versatility’’ of these materials as solid sorbents

doi:10.1007/s11705-022-2187-6

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (11) : 1632-1642 https://doi.org/10.1007/s11705-022-2187-6

RESEARCH ARTICLE

A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications for the ‘‘versatility’’ of these materials as solid sorbents

Xiyuan Bu¹, Ming Tian^1,², Hongqing Wang², Lin Wang¹, Liyong Yuan¹(

), Weiqun Shi¹

¹. Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
². School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China

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Abstract

Although metal–organic frameworks offer a new platform for developing versatile sorption materials, yet coordinating the functionality, structure and component of these materials remains a great challenge. It depends on a comprehensive knowledge of a “real sorption mechanism”. Herein, a ternary mechanism for U(VI) uptake in metal–organic frameworks was reported. Analogous MIL-100s (Al, Fe, Cr) were prepared and studied for their ability to sequestrate U(VI) from aqueous solutions. As a result, MIL-100(Al) performed the best among the tested materials, and MIL-100(Cr) performed the worst. The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(VI) uptake in the three metal–organic frameworks involves different mechanisms. Specifically, hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s (Al, Fe) by exchanging with hydrogen ions of terminal hydroxyl groups (Al-OH₂, Fe-OH₂), and/or, hydrated uranyl ions are bound directly to Al(III) center in MIL-100(Al) through a strong inner-sphere coordination. For MIL-100(Cr), however, the U(VI) uptake is attributed to electrostatic attraction. Besides, the sorption mechanism is also pH and ionic strength dependent. The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism, which helps to construct effective metal–organic frameworks-based sorbents for water purification.

Keywords U(VI) metal–organic frameworks adsorption mechanism metal node

Corresponding Author(s): Liyong Yuan

Online First Date: 28 September 2022 Issue Date: 13 December 2022

Cite this article:

Xiyuan Bu,Ming Tian,Hongqing Wang, et al. A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications for the ‘‘versatility’’ of these materials as solid sorbents[J]. Front. Chem. Sci. Eng., 2022, 16(11): 1632-1642.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2187-6
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I11/1632

Fig.1 Characterizations of the MIL-100 samples. (a) PXRD patterns; (b) TGA curves; (c) N₂ adsorption and desorption isotherms.

Fig.2 The U(VI) uptake in MOFs. (a) Bar graph illustrating the adsorption capacities in several analogous MIL-MOFs (pH = 5 ± 0.1; t = 360 min; m_sorbent/V_solution = 0.4 mg·mL^–1; [U]_initial = 100 mg·L^–1). (b) pH dependence (t = 360 min; m_sorbent/V_solution = 0.4 mg·mL^–1; [U]_initial = 100 mg·L^–1). (c) Sorption kinetics (pH = 5 ± 0.1; m_sorbent/V_solution = 0.4 mg·mL^–1; [U]_initial = 100 mg·L^–1). (d) Sorption isotherms (pH = 5 ± 0.1; t = 360 min; m_sorbent/V_solution = 0.4 mg·mL^–1).

Fig.3 (a) Effect of ionic strength (pH = 5 ± 0.1; t = 360 min; m_sorbent/V_solution = 0.4 mg·mL^–1; [U]_initial = 100 mg·L^–1); (b) competing cations on U(VI) uptake in MIL-100s (Al, Fe, Cr). The concentration of all metal ions was 0.5 mmol·L^–1. m_sorbent/V_solution = 0.4 mg·mL^–1; pH = 5 ± 0.1;t = 360 min.

Fig.4 (a) Zeta Potential of MIL-100; (b) ²⁷Al NMR spectra of pristine MIL-100(Al) (dark line) and after uranyl ion adsorption (red line); (c) fitting line of ²⁷Al NMR spectra of pristine MIL-100(Al); (d) after adsorption of U(VI).

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