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具有配位不饱和位点的 MIL-101(Fe) 增强了活化过硫酸盐降解有机污染物的催化活性。

Enhanced catalytic activity of MIL-101(Fe) with coordinatively unsaturated sites for activating persulfate to degrade organic pollutants.

机构信息

School of Water Conservancy and Environment, University of Jinan, Jinan, 250022, China.

Zhonglu Environmental and Engineering Assessment Center of Shandong Province, Jinan, 250022, China.

出版信息

Environ Sci Pollut Res Int. 2020 May;27(14):17194-17204. doi: 10.1007/s11356-020-08316-z. Epub 2020 Mar 9.

Abstract

In this work, four novel defective MIL-101(Fe) catalysts with coordinatively unsaturated sites were successfully prepared via a facile synthesis strategy by employing benzoic acid, acetic acid, oxalic acid, or citric acid as a modulator. The modified catalysts were demonstrated the existence of defects in the parent framework by a series of characterizations. As compared to the initial MIL-101(Fe), the electronic structure of defective MIL-101(Fe) catalyst was effectively adjusted; meanwhile, the coordinatively unsaturated Fe sites were efficiently generated and the pore sizes were enlarged. Besides, the defective MIL-101(Fe) catalysts exhibited excellent catalytic performance for rhodamine B degradation by persulfate activation. To be specific, the degradation rates of rhodamine B increased from 58.70 to 94.05%, 86.11%, 78.70%, and 82.62%, respectively. The defective MIL-101(Fe) with coordinatively unsaturated sites showed good reusability and stability, and the probable catalytic mechanism was also investigated.

摘要

在这项工作中,通过一种简便的合成策略,成功制备了四种具有配位不饱和位点的新型缺陷 MIL-101(Fe) 催化剂,分别使用苯甲酸、乙酸、草酸或柠檬酸作为调节剂。通过一系列的表征证明了改性催化剂在母体骨架中存在缺陷。与初始的 MIL-101(Fe)相比,缺陷 MIL-101(Fe)催化剂的电子结构得到了有效调节;同时,有效生成了配位不饱和的 Fe 位,并扩大了孔径。此外,缺陷 MIL-101(Fe)催化剂在过硫酸盐活化下对罗丹明 B 的降解表现出优异的催化性能。具体而言,罗丹明 B 的降解率分别提高了 58.70%、86.11%、78.70%和 82.62%。具有配位不饱和位点的缺陷 MIL-101(Fe)表现出良好的可重复使用性和稳定性,并且还研究了可能的催化机制。

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