Photocatalytic degradation of multiple-organic-pollutant under visible light by graphene oxide modified composite: degradation pathway, DFT calculation and mechanism

IF 8.4 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Journal of Environmental Management Pub Date : 2023-09-29 DOI:10.1016/j.jenvman.2023.119128
Qiansu Ma , Jie Ming , Xiang Sun , Hongjian Zhang , Guangqi An , Naoki Kawazoe , Guoping Chen , Yingnan Yang
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Abstract

Wastewater containing antibiotics, organic dyes, and waterborne bacteria is a severe threat to human health and the environment. Amoxicillin has a slow metabolism rate in humans. Methylene blue is mutagenic and carcinogenic. In addition, Salmonella causes serious diarrhea. In this study, an effective 2D/2D photocatalyst with excellent elimination of these pollutants was fabricated by combining graphene oxide (GO), Bi2WO6, BiPO4 and Ag species. GO was applied at varying loading contents (0.8, 1.6, 2.4, 3.2 wt%) to improve the properties of the photocatalyst toward the removal of representative pollutants. The chemical structures, morphology, light absorption and charge mobility were investigated by different GO loading samples. The results indicated that when the wt% of GO was 2.4%, the photocatalyst showed excellent photocatalytic properties and removal rates for typical pollutants. Amoxicillin and methylene blue were mineralized into CO2, H2O, and small molecules, while Salmonella was disinfected with excellent photocatalytic efficiency. Furthermore, the possible photodecomposition pathways of amoxicillin and methylene blue were proposed by DFT calculations and intermediates identified by LCMS. The mechanism of the photocatalytic process was investigated by radical trapping experiments, ESR spectroscopy, and Motty-Schottky plots. The free radicals could be produced constantly during the photocatalytic process, leading to mineralization of amoxicillin and methylene blue, and disinfection of Salmonella. In this work, a new perspective on GO modified Bi2WO6 with different loading contents and the degradation pathways of antibiotics and dyes was proposed.

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氧化石墨烯修饰复合材料在可见光下对多种有机污染物的光催化降解:降解途径、DFT计算和机理。
含有抗生素、有机染料和水性细菌的废水严重威胁着人类健康和环境。阿莫西林在人体内的新陈代谢速度较慢。亚甲基蓝具有诱变性和致癌性。此外,沙门氏菌会引起严重的腹泻。在本研究中,通过将氧化石墨烯(GO)、Bi2WO6、BiPO4和Ag物种结合,制备了一种有效的2D/2D光催化剂,该光催化剂具有优异的去除这些污染物的性能。在不同的负载量(0.8、1.6、2.4、3.2wt%)下施加GO,以改善光催化剂的性能,去除代表性污染物。研究了不同GO负载样品的化学结构、形貌、光吸收和电荷迁移率。结果表明,当GO的wt%为2.4%时,光催化剂表现出优异的光催化性能和对典型污染物的去除率。阿莫西林和亚甲基蓝被矿化成CO2、H2O和小分子,而沙门氏菌则以优异的光催化效率被消毒。此外,通过DFT计算和LCMS鉴定了阿莫西林和亚甲基蓝的可能光分解途径。通过自由基捕获实验、ESR光谱和Motty-Schottky图研究了光催化过程的机理。在光催化过程中,自由基可以不断产生,导致阿莫西林和亚甲基蓝的矿化,以及沙门氏菌的消毒。本工作对不同负载量的GO改性Bi2WO6及其对抗生素和染料的降解途径提出了新的看法。
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来源期刊
Journal of Environmental Management
Journal of Environmental Management 环境科学-环境科学
CiteScore
13.70
自引率
5.70%
发文量
2477
审稿时长
84 days
期刊介绍: The Journal of Environmental Management is a journal for the publication of peer reviewed, original research for all aspects of management and the managed use of the environment, both natural and man-made.Critical review articles are also welcome; submission of these is strongly encouraged.
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