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具有丰富氧空位的二维受限独立氧化石墨烯复合膜,用于通过过一硫酸盐活化增强有机污染物去除

2D confinement freestanding graphene oxide composite membranes with enriched oxygen vacancies for enhanced organic contaminants removal via peroxymonosulfate activation.

作者信息

Ye Jian, Wang Yi, Li Zhanguo, Yang Dayi, Li Chunxiang, Yan Yongsheng, Dai Jiangdong

机构信息

Institute of Green Chemistry and Chemical Technology, Advanced Chemical Engineering Laboratory of Green Materials and Energy of Jiangsu Province, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.

State Key Laboratory of NBC Protection for Civilian, Beijing 102205, China.

出版信息

J Hazard Mater. 2021 Sep 5;417:126028. doi: 10.1016/j.jhazmat.2021.126028. Epub 2021 May 8.

Abstract

Introducing membrane filtration into advanced oxidation processes to decrease energy and cost consumption has been considered as a promising direction in environmental remediation. In this work, we firstly developed a kind of novel lawn-like FeO@CoFe@nitrogen-doped reduced graphene oxide@carbon nanotube composites (FeCo@GCTs) through in-situ pyrolysis of self-assembly of Prussian blue analogues and GO, followed through a vacuum-assisted filtration strategy to fabricate 2D confinement freestanding GO composite membrane. Electrochemical analysis and H-TPR revealed the superiority of FeCo@GCTs as ideal electron acceptor, and this unique lawn-like structure concentrated active sites with a confined space and enriched oxygen vacancies that realized 98.5% (0.128 min) sulfamethoxazole degradation via peroxymonosulfate activation, and accelerated the reduction of Cr(VI). Owing to the increasing interlayer spacing of GO nanosheets, the permeation flux of FeCo@GCTs/GO membrane has not only been attained to 487.3 L·m·h·bar, which was more than 7.5-fold of GO membrane (64.6 L·m·h·bar), but also achieved the synergistic membrane filtration and catalytic degradation of pollutants. Furthermore, scavenger experiments and EPR tests were conducted to confirm the active radicals, of which SO· and O were responsible for SMX degradation. Therefore, these features demonstrated great potential for the fabricated 2D confinement catalytic membrane with enriched oxygen vacancies in wastewater purification.

摘要

将膜过滤引入高级氧化过程以降低能源和成本消耗,已被视为环境修复领域一个有前景的方向。在这项工作中,我们首先通过普鲁士蓝类似物和氧化石墨烯的自组装原位热解,开发了一种新型的草坪状FeO@CoFe@氮掺杂还原氧化石墨烯@碳纳米管复合材料(FeCo@GCTs),随后通过真空辅助过滤策略制备了二维受限独立式氧化石墨烯复合膜。电化学分析和H-TPR揭示了FeCo@GCTs作为理想电子受体的优越性,这种独特的草坪状结构在受限空间内集中了活性位点并富集了氧空位,通过过一硫酸盐活化实现了98.5%(0.128分钟)的磺胺甲恶唑降解,并加速了Cr(VI)的还原。由于氧化石墨烯纳米片层间距的增加,FeCo@GCTs/GO膜的渗透通量不仅达到了487.3 L·m·h·bar,是氧化石墨烯膜(64.6 L·m·h·bar)的7.5倍多,还实现了污染物的协同膜过滤和催化降解。此外,进行了清除剂实验和电子顺磁共振测试以确认活性自由基,其中SO·和O负责磺胺甲恶唑的降解。因此,这些特性表明所制备的具有富氧空位的二维受限催化膜在废水净化方面具有巨大潜力。

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