Research Progress in the Preparation of Functionalized Mesoporous Silica and Its Application in Adsorption and Separation of Uranium from Water

doi:10.19894/j.issn.1000-0518.220236

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (2): 169-187.DOI: 10.19894/j.issn.1000-0518.220236

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Research Progress in the Preparation of Functionalized Mesoporous Silica and Its Application in Adsorption and Separation of Uranium from Water

Qin ZHANG, Wen-Bin LIU, Li-Jiao FAN, Yu-Ming XIE, Guo-Lin HUANG()

School of Chemistry，Biology and Material Science，East China University of Technology，Nanchang 330013，China

Received:2022-07-08 Accepted:2022-10-28 Published:2023-02-01 Online:2023-02-27
Contact: Guo-Lin HUANG
About author:guolinhuang@sina.com
Supported by:
the National Natural Science Foundation of China(21866005)

Abstract

Abstract:

Uranium is an efficient and clean fuel for nuclear energy， but it inevitably produces uranium-containing wastewater in the nuclear industry. If it is not treated in time and leaked into the environment， it will pose a threat to the health of animals， plants and human beings. Therefore， the separation process of U（Ⅵ） in aqueous solution is urgent based on the perspective of energy recovery and environmental protection. Adsorption techniques have especially attracted attentions because of their advantages on feasibility， efficiency and simple operation. As an ideal adsorbent， functionalized mesoporous silica material has the advantages of large specific surface area， high pore capacity and adsorption capacity. It has a wide range of applications in the field of adsorption and separation for uranium. In this paper， the characterization and adsorption mechanism of U（?Ⅵ?） adsorption in aqueous solutions at home and abroad are reviewed on the basis of functionalized mesoporous silica preparation methods， combined with X-ray photoelectron spectroscopy， Fourier transform infrared spectroscopy， X-ray absorption fine structure spectroscopy， X-ray energy spectrum analysis and Raman spectroscopy. Although there have been encouraging and potential developments in functionalized mesoporous silica adsorbed uranium， the design and mass production of novel multifunctional adsorbents for applications in actual environments remain challenging.

Key words: Mesoporous silica, Functionalization, Uranium, Adsorption, Mechanism

CLC Number:

O615

Qin ZHANG, Wen-Bin LIU, Li-Jiao FAN, Yu-Ming XIE, Guo-Lin HUANG. Research Progress in the Preparation of Functionalized Mesoporous Silica and Its Application in Adsorption and Separation of Uranium from Water[J]. Chinese Journal of Applied Chemistry, 2023, 40(2): 169-187.

Figures/Tables 18

Fig.1 Development milestones of mesoporous silicon and its functionalized materials in U（Ⅵ） adsorption［24-32］

Fig.2 Formation of mesoporous materials by structure-directing agents［38］Note：（a） True liquid-crystal template mechanism；（b） Cooperative liquid-crystal template mechanism

Fig.3 （a-d， f）Scanning electron micrographs（SEM） of rod-shaped， spherical， fibrous， cuboidal， and platelet-shaped mesoporous silicon， respectively［41-44］， and （e） transmission electron micrographs（TEM） of fibrous spherical mesoporous silicon［45］

Fig.4 Schematic diagram of post-grafting modification of mesoporous silica［38］

Fig.5 Schematic diagram of the modification of mesoporous silica by silane bridge method［38］

Fig.6 Schematic diagram of modified mesoporous silica by co-condensation method［38］

Fig.7 PXRD patterns of MMSN and MMSN10N［54］

Fig.8 Preparation process of mesoporous silica with magnetic core-shell structure［55-56，58-59］

Fig.9 Response surface diagram of the effect of initial concentration and pH， initial concentration and temperature on the adsorption of UO22+ from aqueous solution by NH2-MCM-41［67］

Table 1 The adsorption properties and main parameters of some functionalized mesoporous silicon for uranium

Adsorbents	Pore diameter/nm	BET surface area/（m²·g^-1）	Equilibrium time /min	Q_max/ （mg·g^-1）	Isotherm model	Ref.
NP10	2.7	920	30	303	Langmuir model	［26］
DIMs	6.7	—	10	268	Langmuir model	［27］
MCM-SUC	2.3	539	10	807	Langmuir model	［31］
MMSN10N	2.88-	815	360	160	Langmuir model	［54］
MMS-AO	2.2	287.1	120	277.3	Langmuir model	［56］
Fe-MCM-SUC	3-13	233	—	430	Langmuir model	［58］
NH₂-MCM-41	1.9	577	173	435	Langmuir model	［67］
MCM-TEPA	3.86	1052	30	454	Langmuir model	［68］
SBA-15-N₂C₁	6.1	267	30	573	Langmuir model	［69］
PFG-MSs	4.6	1.5	60	207.6	Freundlich model	［71］
SMS-Ph	7.73	4.28	60	820.7	Freundlich model	［72］
Fe₃O₄@SiO₂-AO	—	—	120	104.96	Langmuir model	［75］
AO-MCM-41	—	—	40	442.3	Temkin and Freundlich	［76］
Ami-MSN	0.619	676	150	200.41	Langmuir model	［77］
MCM-41-AO	—	—	90	384.59	Langmuir model	［78］
MCC/MS-AO	2.85	358.45	90	315.46	Langmuir model	［82］
Al/MS-AO	0.75	308.89	180	328.68	Langmuir model	［83］

Fig.10 （A） FT-IR spectra of SA， aMSP， and aMSP/SA before and after adsorption；（B） XPS spectra for aMSP/SA before and after adsorption；（C） XPS spectra of curve fitted N1s of aMSP/SA before and after adsorption；（D） backscattered electron image of aMSP/SA after adsorption［87］

Table 2 Sample surface area element composition （EDS analysis）（only elements greater than 0.1% are listed）

Atom.c/%	O	Si	Cl	Ca	U
aMSP/SA	70.0	14.9	1.9	11.5	Not detected
aMSP/SA-U	73.3	17.6	6.1	Not detected	3.0

Fig.11 Mechanism of aMSP/SA interaction with U（Ⅵ）［87］

Fig.12 （A）FT-IR spectra and difference spectra obtained for OMS（a） and OMS-P（b） in contact with U（Ⅵ） solutions of various uranium initial/total concentrations；（B）Raman spectra of OMS-P and OMS after U（?Ⅵ） adsorption at different initial/total U（Ⅵ） concentration［92］

Fig.13 Mechanism of adsorption of uranium by phosphonic acid-functionalized mesoporous silicon material［71，88］

Fig. 14 （a）XPS spectra of MCM-41-AO-40% and MCM-41-AO-40%-U；（b）High resolution spectra of U4f；（c）N1s and（d）O1s core-level spectra of MCM-41-AO-40% and MCM-41-AO-40%-U［78］

Fig.15 FT-IR spectra（a） and EDS patterns（b） of MCM-41-40%-AO before and after adsorption of U（Ⅵ）［78］

Fig.16 Action mechanism diagram of amidoxime chelating uranyl ion［78］

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Research Progress in the Preparation of Functionalized Mesoporous Silica and Its Application in Adsorption and Separation of Uranium from Water

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