Layered Metal Organic Framework for Effective Removal of 137Cs from Aqueous Solution

doi:10.15541/jim20190434

Abstract

Abstract:

¹³⁷Cs is one of the most intractable β-emitters which is commonly generated from nuclear weapons test and nuclear power station. Due to the nature of high solubility and mobility, the effective sequestration of ¹³⁷Cs ⁺ from radioactive waste solution is considered as a long-term challenge. In this work, a two-dimensional layered anion framework material (SZ-6) was synthesized through conventional solvothermal reaction and the Cs ⁺ removal properties were systematically investigated. Single Crystal X-ray Diffraction (SCXRD) analysis revealed that SZ-6 adopts layer packed structure with large tetramethylammonium cations loaded between the layers which is greatly beneficial to cation exchange process. Powder X-ray Diffraction (XRD) and Scanning Electron Microscope (SEM) confirmed the material with high purity and excellent hydrolytic stability. Batch experiments were used to investigate the adsorption behavior towards Cs ⁺ in aqueous solutions. The adsorption kinetics of SZ-6 could be achieved within 5 min, which is currently one of the fastest sorbents for the removal of Cs ⁺. Meanwhile, SZ-6 exhibits superior decontamination capability over a wide pH range from 4 to 12. Furthermore, it possesses marked selectivity in the presence of large excess of Na ⁺, K ⁺, Ca ²⁺ competing cations.

Key words: Metal Organic Frameworks, radionuclide, ¹³⁷Cs, adsorption, kinetics

CLC Number:

X591

LI Guodong, JI Guoxun, SUN Xinli, DU Wei, LIU Wei, WANG Shuao. Layered Metal Organic Framework for Effective Removal of ¹³⁷Cs from Aqueous Solution[J]. Journal of Inorganic Materials, 2020, 35(3): 367-372.

Figures/Tables 10

Fig. 1 Crystal structure of SZ-6 (a) Coordination environment of In3+ center; (b) Asymmetric unit of SZ-6; (c ) Layer packed structure of SZ-6 along the a axis; (d) Rhombic channels viewed along the c axis Atom colors: In = cyan, C = anthracite, N = blue, O =red

Fig. 2 Powder XRD patterns of SZ-6

Fig. 3 SEM-EDS analyses of SZ-6 (a) SEM image, (b) Distribution of In; (c) EDS pattern of SZ-6

Fig. 4 Thermogravimetric analysis curve of SZ-6

Fig. 5 PXRD patterns of samples before and after immersed in Cs+ aqueous solutions with different pH

Fig. 6 Uptake kinetics of Cs+ Inset: simulation curve of Pseudo-second-order model

Fig. 7 Sorption isotherm curves of Cs+ by SZ-6 (Solid curve: Langmuir equilibrium isotherm model; Dotted curve: Freundlich equilibrium isotherm model)

Table 1 Fitting parameters of Langmuir model and Freundlich model

Langmuir			Freundlich
q_m/(mg·g^-1)	K_L/(mg·g^-1)	R²	k_F/(mg·g^-1)	n	R²
140.005	0.024	0.997	20.368	3.295	0.844

Fig. 8 Effect of pH of solution on the adsorption of Cs+ by SZ-6

Table 2 Effect of Na+, K+, Ca2+ on the removal of Cs+ by SZ-6

Competing cation		Cs⁺/Na⁺	Cs⁺/K⁺	Cs⁺/Ca²⁺
Solid/Liquid /(g•L^-1)		2	2	5
Cs⁺ removal/%	MR=1 : 1	87.2	84.7	91.2
	MR=1 : 10	84.2	75.7	90.1
	MR=1 : 20	75.8	65.5	85
	MR=1 : 30	70.3	59	73.7
	MR=1 : 50	63.5	49.3	65.7

References 21

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Layered Metal Organic Framework for Effective Removal of ¹³⁷Cs from Aqueous Solution

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