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通过 MOF 衍生的 FeCo/C 加速电子转移过程,提高抗生素污染物在非均相电芬顿体系中的降解性能。

Accelerated electron transfer process via MOF-derived FeCo/C for enhanced degradation of antibiotic contaminants towards heterogeneous electro-Fenton system.

机构信息

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, PR China; National Engineering Research Center of Urban Water Resources Co., Ltd., Harbin Institute of Technology, Harbin 150090, PR China.

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, PR China.

出版信息

Chemosphere. 2023 Sep;335:138994. doi: 10.1016/j.chemosphere.2023.138994. Epub 2023 May 19.

DOI:10.1016/j.chemosphere.2023.138994
PMID:37211168
Abstract

The Fe(III) to Fe(II) process limits the rate of the electro-Fenton system. In this study, MIL-101(Fe) derived porous carbon skeleton-coated FeCo bimetallic catalyst Fe/Co@PC-700 was prepared as a heterogeneous electro-Fenton (EF) catalytic process. The experimental results showed its good performance in catalytic removal of antibiotic contaminants, the rate constant of tetracycline (TC) degradation catalyzed by Fe/Co@PC-700 was 8.93 times higher than that of Fe@PC-700 under the pH conditions of raw water (pH = 5.86), exhibited good removal of TC, oxytetracycline (OTC), hygromycin (CTC), chloramphenicol (CAP) and ciprofloxacin (CIP). It was shown that the introduction of Co promoted more Fe production, allowing the material to exhibit faster Fe(III)/Fe(II) cycling rates. O and high-priced metal oxygen species were identified as the main active species of the system, in addition to the analysis of possible degradation pathways and toxicity of intermediates of TC. Finally, the stability and adaptability of Fe/Co@PC-700 and EF systems to different water matrices were evaluated, showing that Fe/Co@PC-700 was easy to recover and could be applied to different water matrices. This study provides a reference for the design and system application of heterogeneous EF catalysts.

摘要

三价铁到二价铁的过程限制了电芬顿体系的速率。在本研究中,制备了 MIL-101(Fe)衍生的多孔碳骨架包覆的 FeCo 双金属催化剂 Fe/Co@PC-700,作为一种非均相电芬顿(EF)催化过程。实验结果表明,它在催化去除抗生素污染物方面表现出良好的性能,在原水 pH 值(pH=5.86)条件下,Fe/Co@PC-700 催化四环素(TC)降解的速率常数比 Fe@PC-700 高 8.93 倍,对 TC、土霉素(OTC)、潮霉素(CTC)、氯霉素(CAP)和环丙沙星(CIP)具有良好的去除效果。结果表明,Co 的引入促进了更多的 Fe 生成,使材料表现出更快的 Fe(III)/Fe(II)循环速率。此外,还确定了 O 和高价金属氧物种是该体系的主要活性物质,同时分析了 TC 的可能降解途径和中间体的毒性。最后,评估了 Fe/Co@PC-700 和 EF 系统对不同水基质的稳定性和适应性,结果表明 Fe/Co@PC-700 易于回收,可应用于不同的水基质。本研究为非均相 EF 催化剂的设计和系统应用提供了参考。

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