State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, PR China.
State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, PR China.
J Hazard Mater. 2022 Feb 15;424(Pt A):127387. doi: 10.1016/j.jhazmat.2021.127387. Epub 2021 Sep 30.
In the conventional Fenton system, the relatively low efficiency of Fe (II) regeneration is a significant drawback. To address this shortcoming, a novel floating Z-scheme photo-Fenton catalyst FeMoO/g-CN/EP was prepared by a facile dip-calcination method, in which iron and molybdenum oxides with mixed valence states (FeMoO) and graphitic carbon nitride (g-CN) were loaded on the expanded perlite. The removal efficiencies reached the maximum at 98.0%, 93.1% and 97.1% for tetracycline, oxytetracycline and chlortetracycline, respectively, after 60 min dark adsorption and 60 min photo-Fenton process. The aid of dual ion (Fe and Mo) synergy system and photoreduction by Z-scheme photocatalyst enhanced the Fe (II) regeneration, resulting in the excellent performance. Radical scavenger experiment, electron spin resonance spectra (ESR) and X-ray photoelectron spectra (XPS) were used to confirm the mechanism of free radicals' formation and Fe/Mo redox cycling. ·OH, ·O and O played important roles in the pollutant's degradation, while the generation of ·O was enhanced due to the floatability in this system. The possible degradation pathways of TC were put forward according to the results of mass spectrum and Orbital-Weighted Fukui Function. Overall, this work provides new insights on the cooperation between iron-based mix oxides and semiconductor in the photo-Fenton system.
在传统的芬顿体系中，Fe（II）的再生效率相对较低，这是一个显著的缺点。为了解决这个缺点，通过一种简便的浸渍-煅烧方法制备了一种新型的漂浮 Z 型光芬顿催化剂 FeMoO/g-CN/EP，其中具有混合价态的铁和钼氧化物（FeMoO）和石墨相氮化碳（g-CN）负载在膨胀珍珠岩上。经过 60 分钟的暗吸附和 60 分钟的光芬顿过程，四环素、土霉素和金霉素的去除效率分别达到了最大的 98.0%、93.1%和 97.1%。双离子（Fe 和 Mo）协同体系和 Z 型光催化剂的光还原辅助增强了 Fe（II）的再生，从而表现出优异的性能。自由基捕获实验、电子自旋共振谱（ESR）和 X 射线光电子能谱（XPS）用于确认自由基形成和 Fe/Mo 氧化还原循环的机制。·OH、·O 和 O 在污染物降解中起重要作用，而由于体系的漂浮性，·O 的生成得到增强。根据质谱和轨道加权 Fukui 函数的结果，提出了 TC 的可能降解途径。总的来说，这项工作为铁基混合氧化物和半导体在光芬顿体系中的合作提供了新的见解。
