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以CuFeO/MWCNTs作为过一硫酸盐的非均相催化剂时硫酸根自由基诱导的甲氧苄啶转化:机理与反应途径

Sulfate radical-induced transformation of trimethoprim with CuFeO/MWCNTs as a heterogeneous catalyst of peroxymonosulfate: mechanisms and reaction pathways.

作者信息

Kong Jing, Li Ruobai, Wang Fengliang, Chen Ping, Liu Haijin, Liu Guoguang, Lv Wenying

机构信息

School of Environmental Science and Engineering, Guangdong University of Technology Guangzhou 510006 China

School of Environment, Tsinghua University Beijing 100084 China.

出版信息

RSC Adv. 2018 Jul 10;8(44):24787-24795. doi: 10.1039/c8ra04103b. eCollection 2018 Jul 9.

DOI:10.1039/c8ra04103b
PMID:35542124
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9082366/
Abstract

Trimethoprim (TMP), a typical antibiotic pharmaceutical, has received extensive attention due to its potential biotoxicity. In this study, CuFeO, which was used to decorate MWCNTs a sol-gel combustion synthesis method, was introduced to generate powerful radicals from peroxymonosulfate (PMS) for TMP degradation in an aqueous solution. The results showed that almost 90% of TMP was degraded within 24 min with the addition of 0.6 mM PMS and 0.2 g L CuFeO/MWCNTs. The degradation rate was enhanced with the increase in initial PMS doses, catalyst loading and pH. A fairly low leaching of Cu and Fe was observed during the reaction, indicating the high potential recyclability and stability of CuFeO/MWCNTs. Electron paramagnetic resonance analysis confirmed that the CuFeO/MWCNT-PMS system had the capacity to generate ·OH and SO˙, whereas quenching experiments further confirmed that the catalytic reaction was dominated by SO˙. A total of 11 intermediate products of TMP was detected mass spectrometry, and different transformation pathways were further proposed. Overall, this study showed a systematic evaluation regarding the degradation process of TMP by the CuFeO/MWCNT-PMS system.

摘要

甲氧苄啶(TMP)是一种典型的抗生素药物,因其潜在的生物毒性而受到广泛关注。在本研究中,采用溶胶-凝胶燃烧合成法制备的用于修饰多壁碳纳米管(MWCNTs)的CuFeO,被引入以从过一硫酸盐(PMS)中产生强自由基,用于水溶液中TMP的降解。结果表明,添加0.6 mM PMS和0.2 g/L CuFeO/MWCNTs时,在24分钟内几乎90%的TMP被降解。随着初始PMS剂量、催化剂负载量和pH值的增加,降解速率提高。反应过程中观察到Cu和Fe的浸出量相当低,表明CuFeO/MWCNTs具有很高的潜在可回收性和稳定性。电子顺磁共振分析证实,CuFeO/MWCNT-PMS体系有能力产生·OH和SO˙,而猝灭实验进一步证实催化反应以SO˙为主导。通过质谱检测到TMP共有11种中间产物,并进一步提出了不同的转化途径。总体而言,本研究对CuFeO/MWCNT-PMS体系降解TMP的过程进行了系统评估。

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