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

过硫酸盐 光催化 催化作用 化学 光化学 密度泛函理论 材料科学 可见光谱 电子顺磁共振 激进的 化学工程 金属有机骨架 漫反射红外傅里叶变换 X射线光电子能谱 物理化学 有机化学 光电子学 吸附 计算化学 工程类 物理 核磁共振
作者
Ning Liu,Jinxing Wu,Fuhao Fei,Jianqiu Lei,Wenyan Shi,Guixiang Quan,Shuai Zeng,Xiaodong Zhang,Liang Tang
出处
期刊:Journal of Colloid and Interface Science [Elsevier]
卷期号:612: 1-12 被引量:79
标识
DOI:10.1016/j.jcis.2021.12.142
摘要

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-, SO42-, and NO3- all inhibited the degradation of IBP. X-ray photoelectron spectroscopy (XPS) showed that M88B1 possessed more Fe2+ 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 SO4-•, •OH, O2-•, and 1O2 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.
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