Removal of Radionuclides by Metal-organic Framework-based Materials

Xiang-Xue WANG; Shu-Jun YU; Xiang-Ke WANG; [in Chinese]; [in Chinese]; [in Chinese]

doi:10.15541/jim20180211

Journals >Journal of Inorganic Materials >Volume 34 >Issue 1 >Page 17 > Article

Journal of Inorganic Materials
Vol. 34, Issue 1, 17 (2019)

Removal of Radionuclides by Metal-organic Framework-based Materials

Xiang-Xue WANG, Shu-Jun YU, Xiang-Ke WANG, [in Chinese], [in Chinese], and [in Chinese]

Author Affiliations

College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China

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DOI: 10.15541/jim20180211 Cite this Article

Xiang-Xue WANG, Shu-Jun YU, Xiang-Ke WANG, [in Chinese], [in Chinese], [in Chinese]. Removal of Radionuclides by Metal-organic Framework-based Materials[J]. Journal of Inorganic Materials, 2019, 34(1): 17 Copy Citation Text

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(1) SEM images, (2) XRD patterns, (3) FT-IR spectra, (4) N2 sorption isotherms[26] of MIL-101 and its amino derivatives, (a) MIL-101; (b) MIL-101-NH2; (c) MIL-101-ED; (d) MIL-101-DETA

. (1) SEM images, (2) XRD patterns, (3) FT-IR spectra, (4) N₂ sorption isotherms^[26] of MIL-101 and its amino derivatives, (a) MIL-101; (b) MIL-101-NH₂; (c) MIL-101-ED; (d) MIL-101-DETA

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(a) UV-Vis absorption spectra of TcO4- during the anion exchange; (b) Sorption kinetics of TcO4- by SCU-101 compared with Purolite A530E and A532E; (c) Sorption isotherms of ReO4- by SCU-101, Mg-Al-LDH, and NDTB-1; (d) Effect of competing anions on the removal percentage of TcO4- by SCU-101; (e) Effect of SO42- on the anion exchange of ReO4- by SCU-101; (f) Removal percentage of ReO4- after irradiation as compared with the original SCU-101 sample[28]

. (a) UV-Vis absorption spectra of TcO₄^- during the anion exchange; (b) Sorption kinetics of TcO₄^- by SCU-101 compared with Purolite A530E and A532E; (c) Sorption isotherms of ReO₄^- by SCU-101, Mg-Al-LDH, and NDTB-1; (d) Effect of competing anions on the removal percentage of TcO₄^- by SCU-101; (e) Effect of SO₄^2- on the anion exchange of ReO₄^- by SCU-101; (f) Removal percentage of ReO₄^- after irradiation as compared with the original SCU-101 sample^[28]

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. Linear pseudo-first-order kinetic (a), pseudo-second-order (b), intraparticle diffusion (c) and elovich equation (d) for adsorption of Cs⁺ on MOF/KNiFC and MOF/Fe₃O₄/KNiFC^[44]; (e) Isotherm model of U(VI) adsorption on UiO-66 (inset) and GO-COOH/UiO-66 composites; (f) Langmuir model, (g) Freundlich model, and (h) Dubinin-Radushkevich model^[30]

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. (a) Comparison of experimental U L₃-edge XANES spectra for pristine MIL-101(Cr), and different ED contents grafting ED-MIL-101(Cr) samples after the adsorption of U(VI), (b) Experimental Fourier transform of the U L₃-edge EXAFS data for different samples and their corresponding fits^[54]

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. MD simulations on the process of uranyl sorption into SZ-2. The top (a) and side (b) view of the simulation system-1 (uranyl cation approaching along the c axis); (c) The final snapshot (at t ¼ 100 ns) of run 1 (out of total 6) to show the importance of equatorial water of uranyl cation in mediating its binding to the SZ-2 (the blue dash line indication the hydrogen bond between equatorial water molecules and the dangling hydrogen bond acceptors); (d) Time evolution of the electrostatic and vdW interaction energies of uranyl cation with SZ-2 and water; (e) The number of equatorial water molecules of uranyl cation (pink curve) and the number of hydrogen bonds formed between equatorial coordinating water molecules and other acceptors (including F and O in main framework) as the function of simulation time^[58]

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Adsorbents	Radionuclides	(m/V)/(g·L^-1)	C₀/(mg·L^-1)	t/h	pH	Q_max/(mg·g^-1)	Interaction mechanism	Ref.
MIL-101	U(VI)	0.4	100	2	5.5	20	Surface complexation	[26]
MIL-101-NH₂	U(VI)	0.4	100	2	5.5	90	Surface complexation	[26]
MIL-101-ED	U(VI)	0.4	100	2	5.5	200	Surface complexation	[26]
MIL-101-DETA	U(VI)	0.4	100	2	5.5	350	Surface complexation	[26]
GO-COOH/UiO-66	U(VI)	0.5	95	4	8.0	188	Surface complexation and ion exchange	[30]
SCU-101	Re(IV)	1.0	1000	0.2	-	217	Ion exchange	[28]
SCU-100	Re(IV)	1.0	28	2	-	541	Ion exchange	[29]
UiO-66-(COOH)₂	Th(IV)	0.4	100	6	3.0	350	Surface complexation	[31]
MOF-808-SO₄	Ba(II)	1.0	42	0.1	5.8	131	Surface complexation	[32]
UiO-66-Schiff	Co(II)	0.1	10	5	8.4	256	Surface complexation	[33]
FJSM-InMOF	Sr(II)	2.5	18	12	-	44	Ion exchange	[34]
FJSM-InMOF	Cs(I)	2.5	90	3	-	199	Ion exchange	[34]
LDO-C	U(VI)	0.1	50	4	5.0	354	Surface complexation and ion exchange	[35]
CS@LDH	U(VI)	0.2	41	3	5.0	157	Surface complexation	[36]
GO	Co(II)	0.1	10	4	5.0	44	Surface complexation	[37]
LDH	U(VI)	0.2	50	6	4.5	69	Surface complexation and electrostatic interaction	[38]
Na-montmorillonite	Ni(II)	0.5	10	6	6.0	13	Surface complexation and ion exchange	[39]
Fe₃O₄@TNS	U(VI)	0.2	20	8	5.0	83	Ion exchange	[40]

Table 1. Radionuclides adsorption on different materials

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技术	主要目的	优点	缺点
宏观实验	反应达到平衡所需时间, 最大吸附量, 选择性和影响因素^[30]	非常直观得到实验结果, 方便和有效	无法得到分子和原子水平上的作用机理
XPS分析	元素氧化态、元素种类和几乎所有元素的键合关系(除了H和He)	定量分析、元素组成分析、高表面灵敏度检测(1~10 nm)	在真空中进行的测量, 可能改变样品的性质; 在元素个数比值高于0.05%~ 1.0%条件下进行, 依赖于元素的性质
XAFS分析	氧化态、配位数、原子间键距离以及目标离子周围的离子状态^[54]	特定的元素, 并且总是可以检测到的, 对于研究非晶体材料是有用的; 吸附物种的分析	无法区分原子能相差较小的原子(C、N、O或S、Cl、Mn或Fe)^[59,60]
FT-IR分析	对微米范围内吸附行为的研究(光密度≥10^-5)	灵敏检测官能团和极性键^[61]	定性而不是定量, 灵敏度低
DFT计算	键能、键长、轨道和系统电荷密度^[32,62]	对局部环境的吸附描述和原子级吸附过程的描述^[63]	优化结构之间的能量与长时间模拟结果较不准确
分子动力学模拟	位置、势能和宏观现象的预测^[64]	吸附过程的快照在几秒内发生^[27]	长时间的计算时间, 依赖于计算的性能

Table 2. The main purpose, advantages and disadvantages of main adsorption characterization techniques mentioned above

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