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. 2022 May 12;27(10):3110.
doi: 10.3390/molecules27103110.

Synthesis of Silica-Based Quaternized Adsorption Material and Study on Its Adsorption Behavior for Pu(IV)

Zheng Wang  1 , Meichen Liu  1 , Ling Wang  1 , Zhiyuan Chang  1 , Huibo Li  1
Affiliations

Synthesis of Silica-Based Quaternized Adsorption Material and Study on Its Adsorption Behavior for Pu(IV)

Zheng Wang et al. Molecules. .

Abstract

In this research, we explored the synthesis optimization of the silica-based quaternized adsorption material (SG-VTS-VPQ) and its adsorption behavior for Pu(IV). By optimizing the synthesis process, the grafting amount of 4-vinylpyridine reached 1.25 mmol·g-1. According to the analysis of NMR and XPS, the quaternization rate of pyridine groups reached 91.13%. In the adsorption experiments, the thermodynamic experiment results show that the adsorption of Pu(IV) by SG-VTS-VPQ is more in line with the Langmuir adsorption model and the adsorption type is a typical chemical adsorption; the kinetic results show that adsorption process is more in line with the pseudo first-order kinetic model, and the larger specific surface area of SG-VTS-VPQ plays an important role in the adsorption. The results of the adsorption mechanism show that the adsorption of Pu(IV) by SG-VTS-VPQ is mainly complex anion Pu(NO3)62- and Pu(NO3)5-. This research provides in-depth and detailed ideas for the surface modification and application of porous silica gel, and at the same time provides a new way to develop the direction of the analysis of pretreatment materials in the spent fuel reprocessing field.

Keywords: Pu(IV); adsorption; grafting; reaction mechanism; reprocessing; silica gel.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
Standard curve for Pu(IV) analysis by X-ray fluorescence spectroscopy.
Figure 2
Figure 2
Preparation process of SG-VTS-VPQ and adsorption process of Pu(IV).
Figure 3
Figure 3
Appearance and SEM images of SG (a), SG-VTS (b), SG-VTS-VP (c) and SG-VTS-VPQ (d).
Figure 4
Figure 4
FTIR spectra of the SG (a), SG-VTS (b), SG-VTS-VP (c) and SG-VTS-VPQ (d).
Figure 5
Figure 5
13C-NMR spectra of SG-VTS-VP (a) and SG-VTS-VPQ (b).
Figure 6
Figure 6
Surface morphology of SG-VTS-VP (a) and SG-VTS-VPQ (b).
Figure 7
Figure 7
XPS spectra of SG (a), SG-VTS (b), SG-VTS-VP (c), and SG-VTS-VPQ (d).
Figure 8
Figure 8
The deconvolution of N 1s spectra: SG-VTS-VP (a), SG-VTS-VPQ (b).
Figure 9
Figure 9
Thermogravimetric curve of SG-VTS (a) and SG-VTS-VP (b).
Figure 10
Figure 10
Pore size distribution of SG, SG-VTS, SG-VTS-VP and SG-VTS-VPQ.
Figure 11
Figure 11
Grafting amount varies with 4-VP dosage change.
Figure 12
Figure 12
Grafting amount varies with 4-VP reaction temperature.
Figure 13
Figure 13
Grafting amount varies with initiator dosage.
Figure 14
Figure 14
Orthogonal experiment result.
Figure 15
Figure 15
Effect of [HNO3] and [NO3−] on the adsorption of Pu(IV) by SG-VTS-VPQ.
Figure 16
Figure 16
Effect of HNO3 concentration on the adsorption of Pu(IV) on silica gel and activated carbon.
Figure 17
Figure 17
Adsorption kinetic model for Pu(IV) on SG-VTS-VPQ.
Figure 18
Figure 18
Adsorption isotherm model for Pu(IV) on SG-VTS-VPQ.
Figure 19
Figure 19
Fitting results of Kc and 1/T of Pu(IV).
Figure 20
Figure 20
Fitting results of adsorption mechanism.
Figure 21
Figure 21
Elution curves for uranium and plutonium.
Figure 22
Figure 22
Adsorption of Pu(IV) by SG-VTS-VPQ treated with different concentrations of HNO3. (a) adsorption of Pu(IV) by SG-VTS-VPQ treated with 1 mol·L−1 HNO3; (b) adsorption of Pu(IV) by SG-VTS-VPQ treated with 3 mol·L−1 HNO3; (c) adsorption of Pu(IV) by SG-VTS-VPQ treated with 5 mol·L−1 HNO3; (d) adsorption of Pu(IV) by SG-VTS-VPQ treated with 7 mol·L−1 HNO3; (e) adsorption of Pu(IV) by SG-VTS-VPQ treated with 8 mol·L−1 HNO3; (f) adsorption of Pu(IV) by SG-VTS-VPQ treated with 9 mol·L−1 HNO3.
Figure 23
Figure 23
Infrared spectra of SG-VTS-VPQ treated with different concentrations of HNO3. (a) FTIR of SG-VTS-VPQ treated with 1 mol·L−1 HNO3; (b) FTIR of SG-VTS-VPQ treated with 3 mol·L−1 HNO3; (c) FTIR of SG-VTS-VPQ treated with 5 mol·L−1 HNO3; (d) FTIR of SG-VTS-VPQ treated with 7 mol·L−1 HNO3; (e) FTIR of SG-VTS-VPQ treated with 8 mol·L−1 HNO3; (f) FTIR of SG-VTS-VPQ treated with 9 mol·L−1 HNO3.
Figure 24
Figure 24
Pu(IV) adsorption-desorption five elution curves on SG-VTS-VPQ column.
See this image and copyright information in PMC

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