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Ag-exchanged mesoporous chromium terephthalate with sulfonate for removing radioactive methyl iodide at extremely low concentrations in humid environments
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-04-17 , DOI: 10.1016/j.jhazmat.2021.125904
Ga-Young Cha 1 , Sanil E Sivan 1 , Mijung Lee 2 , Kyung-Ryul Oh 3 , Anil H Valekar 1 , Min-Kun Kim 4 , Heesoo Jung 4 , Do-Young Hong 1 , Young Kyu Hwang 2
Affiliation  

The development of efficient adsorbents to remove radioactive methyl iodide (CH3I) in humid environments is crucial for air purification after pollution by nuclear power plant waste. In this work, we successfully prepared a post-synthetic covalent modified MIL-101 with a sulfonate group followed by the ion-exchange of Ag (I), which is well characterized by diffuse reflectance FT-IR spectroscopy, X-ray photoelectron spectroscopy (XPS) and the hydrophobic index (HI). After modification of the MOFs, we applied functionalized MIL-101 obtained by either one-pot synthesis (MIL-101-SO3Ag) or a post-synthetic modification process (MIL-101-RSO3Ag, R = NH(CH2)3) to remove the CH3I at an extremely low concentration (0.31 ppm) in an environment with very high relative humidity (RH 95%). Enhanced hydrophobicity of the surface-modified MIL-101 was evaluated by examining the HI with the competitive adsorption of water and cyclohexane vapor, with a high surface area maintained, as confirmed by Ar physisorption. Interestingly, the post-synthetically modified MIL-101-RSO3Ag showed exceptional adsorption performance as determined by its decontamination factor (DF = 195,350) at 303 K and RH 95%. This performance was in comparison to Ag (I)-exchanged 13X zeolite and MIL-101-SO3Ag, which include much higher amounts of Ag. Furthermore, MIL-101-RSO3Ag retained ~94–100% of its fresh adsorbent performance during five cycle repetitions.



中文翻译:

银交换的介孔对苯二甲酸铬与磺酸盐的结合,用于在潮湿环境中以极低的浓度去除放射性碘甲烷

开发有效的吸附剂以去除潮湿环境中的放射性碘甲烷(CH 3 I)对于核电站废料污染后的空气净化至关重要。在这项工作中,我们成功地制备了具有磺酸盐基团的合成后共价修饰的MIL-101,随后进行了银(I)的离子交换,其特征在于漫反射FT-IR光谱,X射线光电子能谱( XPS)和疏水指数(HI)。在对MOF进行修饰后,我们应用了通过一锅法合成(MIL-101-SO 3 Ag)或合成后修饰过程(MIL-101-RSO 3 Ag,R = NH(CH 2)3)移除CH 3I在相对湿度(RH 95%)很高的环境中浓度极低(0.31 ppm)。通过Ar与水和环己烷蒸气的竞争性吸附来检查HI,从而评估表面改性MIL-101的增强的疏水性,并保持较高的表面积,这已通过Ar物理吸附得到了证实。有趣的是,合成后改性的MIL-101-RSO 3 Ag在303 K和RH 95%时表现出优异的吸附性能,这取决于其去污系数(DF = 195,350)。该性能与包含更高量的Ag的Ag(I)交换的13X沸石和MIL-101-SO 3 Ag相比。此外,MIL-101-RSO 3 Ag在五个循环重复过程中保留了约94-100%的新鲜吸附性能。

更新日期:2021-05-08
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