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电化学增强磺胺甲恶唑降解效率通过在镍泡沫阴极上生长的碳嵌入铁激活过一硫酸盐:机制和降解途径。

Electro-enhanced sulfamethoxazole degradation efficiency via carbon embedding iron growing on nickel foam cathode activating peroxymonosulfate: Mechanism and degradation pathway.

机构信息

School of Mechanical Engineering and Automation, Northeastern University, Shenyang 110011, PR China.

School of Mechanical Engineering and Automation, Northeastern University, Shenyang 110011, PR China.

出版信息

J Colloid Interface Sci. 2022 Oct 15;624:24-39. doi: 10.1016/j.jcis.2022.05.141. Epub 2022 May 26.

DOI:10.1016/j.jcis.2022.05.141
PMID:35660892
Abstract

The combination of peroxymonosulfate (PMS) activation by hetero-catalysis and electrolysis (EC) attracted incremental concerns as an efficient antibiotics degradation method. In this work, carbon embedding iron (C@Fe) catalysts growing on nickel foam (NF) composite cathode (C@Fe/NF) was prepared via in-situsolvothermal growth and carbonization method and used to activate PMS toward sulfamethoxazole (SMX) degradation. The EC-[C@Fe/NF(II)]-PMS system exhibited an excellent PMS activation, with 100% SMX removal efficiency achieving within 30 min. Reactive oxygen species (ROS) generation and their roles in SMX degradation were confirmed by quenching experiments and electron paramagnetic resonance. It was found that singlet oxygen (O) and surface-bound radicals were responsible for SMX degradation, and O contributed the most. Furthermore, the possible SMX degradation pathways were proposed on the base of the detected degradation intermediates and density functional theory (DFT) calculation. Toxicity changes were also assessed by the Ecological Structure Activity Relationships (ESAR). This work provides a practicable strategy for synergistically enhancing PMS activation efficiency and promoting antibiotics removal.

摘要

过一硫酸盐(PMS)的异相催化和电解(EC)联合激活引起了人们越来越多的关注,成为一种有效的抗生素降解方法。在这项工作中,通过原位溶剂热生长和碳化方法制备了负载在泡沫镍(NF)复合阴极(C@Fe/NF)上的碳嵌入铁(C@Fe)催化剂,并用于激活 PMS 以降解磺胺甲恶唑(SMX)。EC-[C@Fe/NF(II)]-PMS 体系表现出优异的 PMS 激活性能,在 30 min 内可实现 100%的 SMX 去除效率。通过猝灭实验和电子顺磁共振(EPR)证实了活性氧(ROS)的生成及其在 SMX 降解中的作用。发现单线态氧(O)和表面结合自由基是 SMX 降解的主要原因,其中 O 贡献最大。此外,基于检测到的降解中间产物和密度泛函理论(DFT)计算,提出了可能的 SMX 降解途径。还通过生态结构活性关系(ESAR)评估了毒性变化。这项工作为协同提高 PMS 激活效率和促进抗生素去除提供了一种可行的策略。

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