Engineering Research Center for Hydrogen Energy Materials and Devices, College of Rare Earths, Jiangxi University of Science and Technology, 86 Hong Qi Road, Ganzhou, 341000, PR China.
Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, 86 Hong Qi Road, Ganzhou, 341000, PR China.
Environ Res. 2024 Sep 15;257:119350. doi: 10.1016/j.envres.2024.119350. Epub 2024 Jun 4.
The FeOCl-based photo-Fenton heterojunction catalyst holds great promise for effective water pollution treatment. A novel heterojunction FeOCl/MOF-InS (F/M-I) was fabricated by coating hollow MOF-InS nanoflowers onto the surface of FeOCl. Under the optimal conditions, the maximum photo-Fenton degradation rate constants of FeOCl/MOF-InS for oxytetracycline (OTC) within 20 min is 0.88192 L mg·min, which are 3.2 and 2.5 times that of pure FeOCl (0.27357 L mg·min) and MOF-InS (0.35222 L mg·min). Density functional theory (DFT) results confirm that the electron-rich nature of MOF-InS accelerates the cycle between Fe (III)/Fe (II)of FeOCl, promoting HO adsorption by FeOCl/MOF-InS and generating more hydroxyl radicals (·OH) for pollutant degradation. Based on the results of DFT, combined with the results of the reactive oxidation species scavenger (ROSs), electron paramagnetic resonance (EPR) and Mott-Schottky curves, the separation and transfer behavior of photoexcited charges in FeOCl/MOF-InS heterojunction and the possible photocatalytic degradation mechanism were investigated. Finally, a Z-scheme heterostructure is proposed to elucidate the catalytic mechanism. This study provides a new perspective on designing and synthesizing semiconductor materials for water treatment by photo-Fenton catalysis.
基于 FeOCl 的光芬顿异质结催化剂在有效处理水污染方面具有广阔的应用前景。通过在 FeOCl 表面包覆中空 MOF-InS 纳米花,制备了一种新型异质结 FeOCl/MOF-InS(F/M-I)。在最佳条件下,FeOCl/MOF-InS 对土霉素(OTC)的光芬顿降解速率常数在 20 分钟内达到最大值 0.88192 L mg·min,分别是纯 FeOCl(0.27357 L mg·min)和 MOF-InS(0.35222 L mg·min)的 3.2 倍和 2.5 倍。密度泛函理论(DFT)结果证实,MOF-InS 的富电子性质加速了 FeOCl 中 Fe(III)/Fe(II)的循环,促进了 FeOCl/MOF-InS 对 HO 的吸附,并产生更多的羟基自由基(·OH)用于污染物降解。基于 DFT 的结果,结合反应性氧化物种捕获剂(ROSs)、电子顺磁共振(EPR)和 Mott-Schottky 曲线的结果,研究了 FeOCl/MOF-InS 异质结中光激发电荷的分离和转移行为以及可能的光催化降解机制。最后,提出了一种 Z 型结构来阐明催化机制。本研究为设计和合成用于光芬顿催化水处理的半导体材料提供了新的视角。