Performance and mechanism of peroxymonosulfate heterogeneous activation based on FeII-siderite&dithionite for carbamazepine degradation

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology Pub Date : 2025-02-21 DOI:10.1016/j.seppur.2025.132170

Wei Song , Zhaosheng Lei , Hongze Fang , Caixia Fu , Yan Cang , Yuning Fang , Ruigang Wang , Bin Li , Xing Du , Zhihong Wang , Zhiwei Zhao

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引用次数: 0

Abstract

Sulfate radicals-based advanced oxidation process (SO₄⁻-AOPs) exhibits remarkable efficacy for emerging contaminants (ECs) eradication. In this work, we utilized natural Fe^II-siderite as a catalyst with dithionite (DTN) and peroxymonosulfate (PMS) precursors to engineer the Fe^II-siderite&DTN/PMS system. Carbamazepine (CBZ) elimination efficiency exceeded 90% in 10 min with reactive species of SO₄⁻ and OH, even in the anaerobic condition due to the sufficient oxidation species source from broken peroxy bond. The system generated various radicals (e.g., SO₄⁻, SO₃⁻, OH, and SO₅⁻) through redox cycles involving Fe^II-siderite, DTN, and PMS, with Fe^II/Fe^III interconversion driven by PMS oxidation and DTN reduction. Enhanced electron shuttling and Fe^II/Fe^III interconversion at the phase interface, the rate-limiting step in iron-based AOPs, facilitated PMS activation. CBZ degradation followed four pathways including deacylation, ring-opening oxidation, hydroxylation, decarboxylation, and deketonization, with reactive sites at CBZ-7C and CBZ-8C identified by LC-MS/MS and density functional theory (DFT). Oxygen consumption rate (OCR) toxicity assessments revealed persistent toxicity of intermediates, yet the Fe^II-siderite&DTN/PMS system detoxified them effectively based on T.E.S.T. evaluation. And the system demonstrates potential for ECs remediation, particularly in high salinity waters, due to the significant enhancement of higher Cl⁻ concentrations.

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来源期刊

Separation and Purification Technology 工程技术-工程：化工

CiteScore

14.00

自引率

12.80%

发文量

2347

审稿时长

43 days

期刊介绍： Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.