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新型二维/二维FeS/ACN复合材料增强铁/铁循环用于四环素基废水的快速光芬顿降解

Enhanced Fe/Fe cycle by a novel 2D/2D FeS/ACN composite for rapid photo-Fenton degradation of tetracycline-based wastewater.

作者信息

Wu Caiwen, Huang Shan, Cao Xing, Huang Zexiong, Zhang Yanjuan, Huang Zuqiang, Hu Huayu, Gan Tao

机构信息

School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China; Laibin Inspection and Testing Center, Laibin, 546100, PR China.

School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China.

出版信息

J Environ Manage. 2025 Aug;389:126147. doi: 10.1016/j.jenvman.2025.126147. Epub 2025 Jun 13.

Abstract

Fe-based photo-Fenton process is widely used to remove antibiotic in wastewater, however, the synthesis of efficient and stable catalysts to solve the problems of Fe/Fe ions cycling and iron sludge formation of FeS-based catalysts is challenging. Herein, a strategy combining mechanical activation and pyrolysis was proposed to construct a novel FeS/amorphous carbon nitride (2D/2D FeS/ACN) composite with a two-dimensional (2D) stacked structure, where the FeS and ACN connected by Fe-N bonds. The removal rates of oxytetracycline, tetracycline, and chlorotetracycline over 2D/2D FeS/ACN both surpassed 96.0 % within 30 min in the photo-Fenton system, and the photo-Fenton system exhibited a much higher total organic carbon (TOC) removal than the Fenton and photo systems, giving an improvement of rate constant to 3.0 and 6.5 times, respectively. The excellent performance attributed to the fact that the photogenerated electrons were trapped by the sulfur vacancy and directed to the Fe active site for Fe/Fe cycling via a highly-efficient charge transfer channel (Fe-N), resulting in efficiently circulating Fe to Fe. Moreover, due to the involvement of photogenerated electrons in the reduction of Fe to decrease the consumption of S (S and S), 2D/2D FeS/ACN showed superior stability after five cycles, inhibiting the formation of iron sludge. This work provides a new route for the acceleration of Fe/Fe cycling in Fe-based photo-Fenton process for the efficient treatment of tetracycline-based wastewater.

摘要

铁基光芬顿法被广泛用于去除废水中的抗生素,然而,合成高效稳定的催化剂以解决铁基硫化物催化剂的铁/铁离子循环和铁泥形成问题具有挑战性。在此,提出了一种结合机械活化和热解的策略,构建了一种具有二维(2D)堆叠结构的新型硫化铁/非晶态氮化碳(2D/2D FeS/ACN)复合材料,其中FeS和ACN通过Fe-N键连接。在光芬顿体系中,2D/2D FeS/ACN对土霉素、四环素和金霉素的去除率在30分钟内均超过96.0%,且该光芬顿体系的总有机碳(TOC)去除率比芬顿体系和光体系高得多,速率常数分别提高到3.0倍和6.5倍。优异的性能归因于光生电子被硫空位捕获,并通过高效电荷转移通道(Fe-N)导向Fe活性位点进行Fe/Fe循环,从而实现铁的高效循环。此外,由于光生电子参与铁的还原以减少硫的消耗(S和S),2D/2D FeS/ACN在五个循环后表现出优异的稳定性,抑制了铁泥的形成。这项工作为加速铁基光芬顿法中Fe/Fe循环以高效处理四环素类废水提供了一条新途径。

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