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用于在潮湿环境中极低浓度去除放射性甲基碘的 Ag 交换介孔对苯二甲酸铬磺酸盐。

Ag-exchanged mesoporous chromium terephthalate with sulfonate for removing radioactive methyl iodide at extremely low concentrations in humid environments.

机构信息

Research Center for Nanocatalysts, Korea Research Institute of Chemical Technology (KRICT), Jang-dong, Yuseong, Daejeon 34114, Republic of Korea.

Research Center for Nanocatalysts, Korea Research Institute of Chemical Technology (KRICT), Jang-dong, Yuseong, Daejeon 34114, Republic of Korea; Department of Advanced Materials and Chemical Engineering, University of Science and Technology (UST), Gajeong-dong, Yuseong, Daejeon 34113, Republic of Korea.

出版信息

J Hazard Mater. 2021 Sep 5;417:125904. doi: 10.1016/j.jhazmat.2021.125904. Epub 2021 Apr 17.

Abstract

The development of efficient adsorbents to remove radioactive methyl iodide (CHI) 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-SOAg) or a post-synthetic modification process (MIL-101-RSOAg, R = NH(CH)) to remove the CHI 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-RSOAg 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-SOAg, which include much higher amounts of Ag. Furthermore, MIL-101-RSOAg retained ~94-100% of its fresh adsorbent performance during five cycle repetitions.

摘要

在核废料污染后,开发高效的吸附剂去除潮湿环境中的放射性甲基碘(CHI)对于空气净化至关重要。在这项工作中,我们成功地制备了一种磺酸基后合成共价修饰的 MIL-101,随后进行了 Ag(I)的离子交换,通过漫反射傅里叶变换红外光谱、X 射线光电子能谱(XPS)和疏水性指数(HI)对其进行了很好的表征。在 MOFs 修饰后,我们应用了通过一锅合成法(MIL-101-SOAg)或后合成修饰法(MIL-101-RSOAg,R = NH(CH))获得的功能化 MIL-101,以去除在非常高的相对湿度(RH 95%)环境中极低浓度(0.31 ppm)的 CHI。通过考察水和环己烷蒸气的竞争吸附对表面修饰的 MIL-101 的疏水性增强情况,用 HI 进行评估,在高比表面积下保持了疏水性,这一点通过 Ar 物理吸附得到了证实。有趣的是,通过 303 K 和 RH 95%下的去污因子(DF = 195350),后合成修饰的 MIL-101-RSOAg 表现出了优异的吸附性能。与包含更多 Ag 的 Ag(I)交换 13X 沸石和 MIL-101-SOAg 相比,MIL-101-RSOAg 的性能有所提高。此外,MIL-101-RSOAg 在五次循环重复中保留了其新鲜吸附剂性能的约 94-100%。

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