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. 2018 Nov 22;8(68):39149-39161.
doi: 10.1039/c8ra07762b. eCollection 2018 Nov 16.

Synthesis and characterization of magnetic mesoporous Fe3O4@mSiO2-DODGA nanoparticles for adsorption of 16 rare earth elements

Jingrui Li  1   2 , Aijun Gong  1   2 , Fukai Li  1   2 , Lina Qiu  1   2 , Weiwei Zhang  1   2 , Ge Gao  1   2 , Yu Liu  1   2 , Jiandi Li  1   2
Affiliations

Synthesis and characterization of magnetic mesoporous Fe3O4@mSiO2-DODGA nanoparticles for adsorption of 16 rare earth elements

Jingrui Li et al. RSC Adv. .

Abstract

In this study, novel magnetic mesoporous Fe3O4@mSiO2-DODGA nanoparticles were prepared for efficiently adsorbing and recycling REEs. Fe3O4@mSiO2-DODGA was characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), vibrating sample magnetometry (VSM), Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA). The adsorption behavior of Fe3O4@mSiO2-DODGA was investigated by ICP-OES. The results showed that the content of DODGA in the adsorbent was 367 μmol g-1. Fe3O4@mSiO2-DODGA exhibited the highest adsorption rates for 15 REEs, except Tm, in a 2 mol L-1 nitric acid solution. Among these elements, the adsorption rates for Nd, Sm, Eu, Dy, Ho, Yb, Lu, Y and Sc ranged from 85.1% to 100.1%. The desorption rates for all 16 REE ions reached their maximum values when 0.01 mol L-1 EDTA was used as the eluent. The desorption rates for Nd, Ce, Sm, Eu, Ho, Yb, Lu, Y, and Sc were 87.7-99.8%. Fe3O4@mSiO2-DODGA had high stability in 2 mol L-1 HNO3 and could be used five times without significant loss of adsorption capacity. Moreover, these nanoparticles had high selectivity, and their adsorption rate was not affected even in a high-concentration solution of a coexisting ion. Therefore, 8 REE ions (Nd, Sm, Eu, Ho, Yb, Lu, Y, and Sc) were selected for the study of adsorption kinetics and adsorption isotherm experiments. It was demonstrated that the values of Q e (equilibrium adsorption capacity) for Nd, Sm, Eu, Ho, Yb, Lu, Y, and Sc were 14.28-60.80 mg g-1. The adsorption of REEs on Fe3O4@mSiO2-DODGA followed the pseudo-second-order kinetic model, Elovich model and Langmuir isotherm model, which indicated that the adsorption process of Fe3O4@mSiO2-DODGA for REEs comprised single-layer adsorption on a non-uniform surface controlled by chemical adsorption. It was concluded that Fe3O4@mSiO2-DODGA represents a new material for the adsorption of REEs in strongly acidic solutions.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Scheme 1
Scheme 1. Preparation of the functionalized Fe3O4 nanoparticles.
Fig. 1
Fig. 1. TEM images of hollow Fe3O4 (a and b), SAED pattern (c), and TEM images of Fe3O4@SiO2 (d) and Fe3O4@mSiO2 (e and f).
Fig. 2
Fig. 2. XRD patterns (A), FT-IR spectra (B), TGA curves (C) and VSM curves (D) of Fe3O4 nanoparticles.
Fig. 3
Fig. 3. Effect of different concentrations of HNO3 on the adsorption rate.
Fig. 4
Fig. 4. Effect of EDTA concentration on desorption rate.
Fig. 5
Fig. 5. Adsorption rates of Fe3O4@mSiO2–DODGA after being immersed in an HNO3 solution for different numbers of days.
Fig. 6
Fig. 6. Adsorption kinetics of 8 REEs.
Fig. 7
Fig. 7. Kinetic plots for Nd as a representative element: (a) pseudo-first-order, (b) pseudo-second-order, (c) intra-particle diffusion, and (d) Elovich models.
Fig. 8
Fig. 8. Adsorption isotherms for the adsorption of REEs on Fe3O4@mSiO2–DODGA.
Fig. 9
Fig. 9. Adsorption model plots for Nd as a representative element: (a) Langmuir, (b) Freundlich, (c) Temkin, and (d) D-R models.
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