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醌基改性 NH-MIL-101(Fe) 复合材料作为氧化还原介体,提高双酚 A 的降解性能。

Quinone-modified NH-MIL-101(Fe) composite as a redox mediator for improved degradation of bisphenol A.

机构信息

School of Resources and Environment, University of Jinan, Jinan, ShanDong Province, China.

出版信息

J Hazard Mater. 2017 Feb 15;324(Pt B):665-672. doi: 10.1016/j.jhazmat.2016.11.040. Epub 2016 Nov 15.

Abstract

A novel quinone-modified metal-organic frameworks NH-MIL-101(Fe) was synthesized using a simple chemical method under mild condition. The introduced 2-anthraquinone sulfonate (AQS) can be covalently modified with NH-MIL-101(Fe) and acts as a redox mediator to enhance the degradation of bisphenol A (BPA) via persulfate activation. The obtained AQS-NH-MIL-101(Fe) was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectra, cyclic voltammetry and electrochemical impedance spectroscopy. AQS-NH-MIL-101(Fe) exhibited better catalytic performance compared with NH-MIL-101(Fe) and NH-MIL-101(Fe) with free AQS (NH-MIL-101(Fe)/AQS). That is, AQS-NH-MIL-101(Fe) was proved to be the most effective in that more than 97.7% of BPA was removed. The degradation rate constants (k) of AQS-NH-MIL-101(Fe) was 9-fold higher than that of NH-MIL-101(Fe) and 7-fold higher than NH-MIL-101(Fe)/AQS, indicating that AQS is a great electron-transfer mediator when modified with NH-MIL-101(Fe). Based on the above results, the possible mechanism of catalytic reaction has been investigated in view of the trapping experiments. In addition, the AQS-NH-MIL-101(Fe) catalyst exhibited excellent stability and can be used several times without significant deterioration in performance.

摘要

一种新型醌改性金属有机骨架 NH-MIL-101(Fe) 是在温和条件下通过简单的化学方法合成的。引入的 2-蒽醌磺酸盐 (AQS) 可以与 NH-MIL-101(Fe) 进行共价修饰,并作为氧化还原介体通过过硫酸盐活化来增强双酚 A (BPA) 的降解。所得到的 AQS-NH-MIL-101(Fe) 通过傅里叶变换红外光谱、X 射线衍射、扫描电子显微镜、X 射线光电子能谱、循环伏安法和电化学阻抗谱进行了表征。与 NH-MIL-101(Fe) 和具有游离 AQS 的 NH-MIL-101(Fe) (NH-MIL-101(Fe)/AQS) 相比,AQS-NH-MIL-101(Fe) 表现出更好的催化性能。也就是说,AQS-NH-MIL-101(Fe) 被证明是最有效的,因为超过 97.7%的 BPA 被去除。AQS-NH-MIL-101(Fe) 的降解速率常数 (k) 比 NH-MIL-101(Fe) 高 9 倍,比 NH-MIL-101(Fe)/AQS 高 7 倍,表明 AQS 是一种很好的电子转移介体当与 NH-MIL-101(Fe) 修饰时。基于上述结果,从捕获实验的角度研究了催化反应的可能机制。此外,AQS-NH-MIL-101(Fe) 催化剂表现出优异的稳定性,可以多次使用而不会显著降低性能。

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