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在模拟可见光下,通过面控制的MIL-88B(Fe)与过硫酸盐的协同作用实现布洛芬的降解。

Ibuprofen degradation by a synergism of facet-controlled MIL-88B(Fe) and persulfate under simulated visible light.

作者信息

Liu Ning, Wu Jinxing, Fei Fuhao, Lei Jianqiu, Shi Wenyan, Quan Guixiang, Zeng Shuai, Zhang Xiaodong, Tang Liang

机构信息

School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai 200093, PR China.

Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, PR China.

出版信息

J Colloid Interface Sci. 2022 Apr 15;612:1-12. doi: 10.1016/j.jcis.2021.12.142. Epub 2021 Dec 25.

Abstract

The photocatalysis/persulfate (PS) hybrid system has proven to be a promising method for degrading organic pollutants from aqueous solutions. In this study, three MIL-88B(Fe) iron-based metal-organic framework (MOF) phases with different facet content were prepared and used both as photocatalysts and catalysts for PS activation to remove ibuprofen (IBP). The results showed that there was a close correlation between the exposed facets and the catalytic activity. MIL-88B(Fe)-1 (M88B1) with exposed {100} facets and proportionally more {101} facets showed the best catalytic activity. The optimum PS dosage used in this study was 60 mg/L. The presence of Cl, SO, and NO all inhibited the degradation of IBP. X-ray photoelectron spectroscopy (XPS) showed that M88B1 possessed more Fe than the other two MIL-88B(Fe) MOF phases, making it easier to generate active radicals through PS activation. The UV-vis diffuse reflectance spectra (DRS), photoluminescence (PL), and electrochemical analysis indicated that M88B1 possessed the highest light absorption, most active sites, and fastest charge transfer ability. Radical scavenging and electron spin resonance (ESR) experiments demonstrated that SO, OH, O, and O species participated in the IBP degradation process. Furthermore, density functional theory (DFT) calculations were performed to identify the crystallographic facets, band structure, and total density of states of MIL-88B(Fe) to further confirm the mechanism of MIL-88B(Fe) as a photocatalyst and a PS activator. This work provides new insights into the synergism between photocatalysis and persulfate activation by facet-controlled MOFs for environmental remediation.

摘要

光催化/过硫酸盐(PS)混合体系已被证明是一种从水溶液中降解有机污染物的有前景的方法。在本研究中,制备了具有不同晶面含量的三种MIL-88B(Fe)铁基金属有机框架(MOF)相,并将其用作光催化剂和PS活化催化剂以去除布洛芬(IBP)。结果表明,暴露的晶面与催化活性之间存在密切相关性。具有暴露的{100}晶面且{101}晶面比例更高的MIL-88B(Fe)-1(M88B1)表现出最佳的催化活性。本研究中使用的最佳PS剂量为60 mg/L。Cl、SO和NO的存在均抑制了IBP的降解。X射线光电子能谱(XPS)表明,M88B1比其他两种MIL-88B(Fe) MOF相具有更多的Fe,这使得它更容易通过PS活化产生活性自由基。紫外可见漫反射光谱(DRS)、光致发光(PL)和电化学分析表明,M88B1具有最高的光吸收、最多的活性位点和最快的电荷转移能力。自由基清除和电子自旋共振(ESR)实验表明,SO、OH、O和O物种参与了IBP的降解过程。此外,进行了密度泛函理论(DFT)计算以确定MIL-88B(Fe)的晶体学晶面、能带结构和态密度,以进一步证实MIL-88B(Fe)作为光催化剂和PS活化剂的机理。这项工作为通过晶面控制的MOF进行光催化和过硫酸盐活化之间的协同作用以实现环境修复提供了新的见解。

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