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铁氮共掺杂珊瑚状空心碳壳用于促进过一硫酸盐活化以高效降解四环素:单线态氧主导的非自由基途径

Fe-N co-doped coral-like hollow carbon shell toward boosting peroxymonosulfate activation for efficient degradation of tetracycline: Singlet oxygen-dominated non-radical pathway.

作者信息

Chen Wenjin, Huang Jin, Shen Yaqian, Zhu Ke, Lei Lele, He Hongmei, Ai Yushi

机构信息

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.

出版信息

J Environ Sci (China). 2023 Apr;126:470-482. doi: 10.1016/j.jes.2022.03.018. Epub 2022 Mar 23.

Abstract

Fe-N co-doped coral-like hollow carbon shell (Fe-N-CS) was synthesized via a simply impregnation-pyrolysis method. The Fe-N-CS showed an excellent ability for activating peroxymonosulfate (PMS), which could degrade about 93.74% tetracycline (20 mg/L) in 12 min. The Fe-N-CS/PMS system exhibited a good anti-interference capacity of various pH, inorganic anions, HA and different water qualities. More importantly, the Fe nanoparticles were anchored uniformly in the carbon layer, effectively limiting the metal leaching. The quenching tests and electron spin resonance (ESR) manifested that non-radical singlet oxygen (O) was the main reactive oxygen species (ROS) for TC degradation. The mechanism study showed that Fe nanoparticles, defect and graphite N played a key role in activating PMS to produce ROS. Moreover, three probable degradation pathways were proposed by using LC-MS measurements. Generally, this work had a new insight for the synthesis of heterogeneous Fe-N-C catalysts in the advanced oxidation process based on PMS.

摘要

通过简单的浸渍-热解方法合成了铁-氮共掺杂的珊瑚状空心碳壳(Fe-N-CS)。Fe-N-CS表现出优异的活化过一硫酸盐(PMS)的能力,在12分钟内可降解约93.74%的四环素(20 mg/L)。Fe-N-CS/PMS体系对各种pH值、无机阴离子、腐殖酸(HA)和不同水质具有良好的抗干扰能力。更重要的是,铁纳米颗粒均匀地锚定在碳层中,有效地限制了金属的浸出。猝灭试验和电子自旋共振(ESR)表明,非自由基单线态氧(O)是四环素降解的主要活性氧物种(ROS)。机理研究表明,铁纳米颗粒、缺陷和石墨态氮在活化PMS产生活性氧方面起关键作用。此外,通过液相色谱-质谱联用(LC-MS)测量提出了三种可能的降解途径。总的来说,这项工作为基于PMS的高级氧化过程中合成非均相铁-氮-碳催化剂提供了新的见解。

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