Boosting photocatalytic degradation of antibiotics: The role of alcohol solvent on the morphology and bandgap structure of FeWO4 used for peroxymonosulfate activation

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Shengyu Jing, Han Li, Huagen Liang, Ruolin Cheng, Angeliki Brouzgou, Panagiotis Tsiakaras
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Abstract

Advanced oxidation process based on persulfate activation has been considered as a proven and effective means of rapidly removing organic pollutants from sewage. However, the low efficiency of heterogeneous catalysts still hinders its widespread application. Herein, FeWO4 synthesized by solvothermal method, using different water/alcohol mixed solvents, is employed to photocatalytically activate peroxymonosulfate (PMS) for antibiotics degradation. Due to differences in solvent polarity, dissolution kinetics and physicochemical properties of different alcohols (ethanol, ethylene glycol, glycerol), the morphology, specific surface area, pore structure, photoelectric properties, band gap structure, and consequently the photocatalytic activity of FeWO4, are significantly affected. It is found that as the alcoholic hydroxyl groups increase, the FeWO4 morphology gradually changes from nanorods to rice-grain-like nanoparticles, accompanied by an increase in specific surface-area and pores, an extension of the reaction-interface and light-absorption area, and an exposure of more active sites. Among them, FeWO4 (DZ:GI = 2:8), synthesized in a deionized water/glycerol mixed solvent with a volume ratio of 2:8, exhibits the highest photocatalytic activity for activating PMS. Within 15 mins, the removal rate of tetracycline (TC) catalyzed by FeWO4 (DZ:GI = 2:8) reaches 100 %. Free radical trapping experiments and electron paramagnetic resonance (EPR) spectra confirm that oxygen singlet (1O2) has a key role in TC degradation. Whereas hydroxyl radicals (•OH), holes (h+), superoxide radicals (•O2), and sulfate radicals (SO4•−) play only a minor role.

Abstract Image

促进抗生素光催化降解:醇溶剂对过氧单硫酸氢氧化铁形态和带隙结构的影响
基于过硫酸盐活化的深度氧化工艺被认为是一种快速去除污水中有机污染物的有效方法。然而,非均相催化剂的低效率仍然阻碍了其广泛应用。本文采用溶剂热法合成FeWO4,采用不同的水/醇混合溶剂,光催化激活过氧单硫酸根(PMS)降解抗生素。由于不同醇类(乙醇、乙二醇、甘油)的溶剂极性、溶解动力学和物理化学性质的差异,对FeWO4的形貌、比表面积、孔结构、光电性能、带隙结构以及光催化活性产生了显著影响。研究发现,随着醇羟基的增加,FeWO4的形貌逐渐由纳米棒转变为米粒状纳米颗粒,同时比表面积和孔洞增大,反应界面和吸光面积扩大,活性位点暴露增多。其中,在体积比为2:8的去离子水/甘油混合溶剂中合成的FeWO4 (DZ:GI = 2:8)对PMS的光催化活性最高。FeWO4 (DZ:GI = 2:8)在15 min内对四环素(TC)的去除率达到100% %。自由基捕获实验和电子顺磁共振(EPR)谱证实氧单线态(1O2)在TC降解中起关键作用。而羟基自由基(•OH)、空穴(h+)、超氧自由基(•O2 -)和硫酸盐自由基(SO4•−)只起次要作用。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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