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钴掺杂石墨相氮化碳作为过氧乙酸降解磺胺甲恶唑的有效催化剂。

Cobalt doped graphitic carbon nitride as an effective catalyst for peracetic acid to degrade sulfamethoxazole.

作者信息

Zhou Runyu, Zhou Gaofeng, Liu Yiqing, Wang Shixiang, Fu Yongsheng

机构信息

Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University Chengdu 611756 China

出版信息

RSC Adv. 2022 May 9;12(22):13810-13819. doi: 10.1039/d2ra00821a. eCollection 2022 May 5.

Abstract

In this study, cobalt doped graphitic carbon nitride (Co-CN) was prepared and applied as a catalyst to activate peracetic acid (PAA) for sulfamethoxazole (SMX) degradation at neutral pH. PAA could be efficiently activated by Co-CN resulting in the efficient degradation of SMX. Characterization results of fresh and used Co-CN suggested that cobalt was successfully doped in graphitic carbon nitride (g-CN) through chemical bonding (Co-N bond) and the surface cobalt species in Co-CN (, [triple bond, length as m-dash]Co(ii) and [triple bond, length as m-dash]Co(iii)) were the main activators for PAA. Organic radicals (, CHC(O)O˙ and CHC(O)OO˙) were proved to be the dominant reactive species for SMX removal in the Co-CN/PAA system by radical scavenging experiments. The increase of cobalt doping content, PAA dosage or Co-CN dosage could accelerate SMX degradation and the neutral condition was highly favorable to SMX removal in Co-CN/PAA system. Co-CN exhibited a good stability and reusability for PAA activation in degrading SMX. Four possible degradation pathways of SMX (, hydroxylation, nitration, bond cleavage and coupling reaction) were proposed in the Co-CN/PAA system according to eight identified transformation products.

摘要

在本研究中,制备了钴掺杂的石墨相氮化碳(Co-CN)并将其用作催化剂,以在中性pH值下活化过氧乙酸(PAA)来降解磺胺甲恶唑(SMX)。Co-CN能够有效活化PAA,从而实现SMX的高效降解。新鲜和使用过的Co-CN的表征结果表明,钴通过化学键合(Co-N键)成功掺杂在石墨相氮化碳(g-CN)中,并且Co-CN中的表面钴物种([三键,长度为m破折号]Co(ii)和[三键,长度为m破折号]Co(iii))是PAA的主要活化剂。通过自由基清除实验证明,有机自由基([三键,长度为m破折号]CHC(O)O˙和[三键,长度为m破折号]CHC(O)OO˙)是Co-CN/PAA体系中去除SMX的主要活性物种。钴掺杂量、PAA用量或Co-CN用量的增加均可加速SMX的降解,并且中性条件对Co-CN/PAA体系中SMX的去除非常有利。Co-CN在降解SMX的PAA活化反应中表现出良好的稳定性和可重复使用性。根据八种已鉴定的转化产物,在Co-CN/PAA体系中提出了SMX的四种可能降解途径([三键,长度为m破折号]羟基化、硝化、键断裂和偶联反应)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3650/9082621/399a78d98efb/d2ra00821a-f1.jpg

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