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氮掺杂多孔碳在单一和二元体系中协同吸附和过硫酸盐活化去除抗生素的动力学和机理。

Kinetics and mechanism of synergistic adsorption and persulfate activation by N-doped porous carbon for antibiotics removals in single and binary solutions.

机构信息

School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia; Centre for Future Materials, University of Southern Queensland, Springfield Central, QLD 4300, Australia.

School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia.

出版信息

J Hazard Mater. 2022 Feb 5;423(Pt A):127083. doi: 10.1016/j.jhazmat.2021.127083. Epub 2021 Aug 30.

Abstract

Porous carbon serves as a green material for efficient wastewater purification by adsorption and advanced oxidation processes. However, a clear understanding of the simultaneous removal of multiple pollutants in water is still ambiguous. Herein, the synergistic effect of adsorption and peroxydisulfate (PS) activation on kinetics and mechanism of removing single and binary antibiotic pollutants, sulfamethoxazole (SMX) and ibuprofen (IBP), from water by biomass-derived N-doped porous carbon was investigated. Our findings suggest that adsorption contributed to efficient removals of SMX/IBP. Comparative quenching experiments and electrochemical analysis demonstrated that hydroxyl (•OH) and sulfate (SO) radicals, as well as singlet oxygen (O) led to the catalytic degradation of SMX, while only O reacted for IBP oxidation. Superoxide ion (O) radicals were not related to SMX/IBP degradation. Electron transfer pathway accounted for PS activation but was not involved in direct SMX/IBP oxidation. Only slight differences were found between the degradation kinetics of SMX and IBP in the binary and single SMX or IBP solutions. This arose from the non-selective effect of adsorption and O attack for SMX/IBP removal, and the weak selective oxidation process of SMX by •OH and SO. This study provides a new viewpoint on the role of adsorption in catalysis and enriches the mechanistic study of multi-component antibiotic degradation.

摘要

多孔碳作为一种绿色材料,通过吸附和高级氧化过程,可有效净化废水。然而,对于水中多种污染物的同时去除,其机制仍不明确。本文研究了生物质衍生的 N 掺杂多孔碳对水中单一组分和双组分抗生素污染物磺胺甲恶唑(SMX)和布洛芬(IBP)的吸附和过一硫酸盐(PS)活化的协同去除动力学和机制。研究结果表明,吸附对 SMX/IBP 的有效去除起主要作用。比较猝灭实验和电化学分析表明,•OH 和 SO 自由基以及单线态氧(O)导致 SMX 的催化降解,而只有 O 用于 IBP 的氧化。超氧离子(O)自由基与 SMX/IBP 降解无关。电子转移途径解释了 PS 的活化,但不涉及 SMX/IBP 的直接氧化。在双组分和单一组分 SMX 或 IBP 溶液中,SMX 和 IBP 的降解动力学仅略有差异。这是由于吸附的非选择性和 O 对 SMX/IBP 去除的攻击作用,以及•OH 和 SO 对 SMX 的弱选择性氧化过程所致。本研究为吸附在催化中的作用提供了新的视角,并丰富了多组分抗生素降解的机理研究。

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