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Enhanced peroxymonosulfate activation by CoFe doped carbon polyhedral nanocages through protecting-etching regulation for ciprofloxacin degradation

文献类型： 外文期刊

作者： Yang, Bowen 1 ; Zhang, Haiqing 2 ; Zhang, Shihan 1 ; Guo, Haixin 3 ; Su, Yaqiong 4 ; Qi, Xinhua 1 ;

作者机构： 1.Nankai Univ, Coll Environm Sci & Engn, 38,Tongyan Rd, Tianjin 300350, Peoples R China

2.Minist Agr & Rural Affairs, Inst Control Agrochem, 22,Maizidian St, Beijing 100125, Peoples R China

3.Chinese Acad Agr Sci, Agroenvironm Protect Inst, 31,Fukang Rd, Tianjin 300191, Peoples R China

4.Xi An Jiao Tong Univ, Engn Res Ctr Energy Storage Mat & Devices Minist E, Natl Innovat Platform Ctr Ind Educ Integrat Energy, Sch Chem, Xian 710049, Peoples R China

关键词： Peroxymonosulfate; Tannic Acid; Nanocages; Density Functional Theory; Degradation mechanism

期刊名称：CHEMICAL ENGINEERING JOURNAL （ 影响因子：13.2； 五年影响因子：13.5 ）

ISSN： 1385-8947

年卷期： 2025 年 521 卷

页码：

收录情况： SCI

摘要： Improving the activation efficiency of peroxymonosulfate (PMS) to produce more radicals is crucial to promote Fenton-like reactions. Herein, hollow carbon polyhedral nanocages-loaded CoFe catalysts via tannic acid etching (TA-CoFe-NC) were prepared based on the metal-ligand exchange mechanism. The magnetic catalyst, with little metal leaching during reaction, achieved the removal efficiency of 95.5 % in ciprofloxacin degradation within 30 min and a first-order kinetic constant of 0.054 min-1 under optimal conditions (0.1 g center dot L-1 catalyst, 0.2 g center dot L-1 PMS, unadjusted pH), a 10.76-fold enhancement compared to the unetched catalyst. By quenching experiments and EPR, 1O2, SO4 center dot- , and center dot OH were proved to be the critical reactive species in degradation process. Density functional theory calculations elucidated the adsorption of PMS and the spontaneous decomposition into center dot OH and SO4 center dot- in catalytic process. High d-band center and low integrated crystal orbital Hamilton population promoted the charge transport and catalytic property. Degradation pathway and toxicity of intermediates were also investigated, and exhibited excellent stability and tolerance to environmental interferences. The rational protecting-etching manipulation by TA helps design novel catalysts with high performance and stability, and facilitates PMS adsorption and interfacial electron transfer to achieve the synergetic stabilization-promotion effect.

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