Activation of PAA by pyrite for the degradation of tetracycline with adjusted pH conditions: The overlooked role of sulfur species

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-12-25 DOI:10.1016/j.seppur.2024.131225
Hongling Dai , Zhen Huang , Chuqiao Wang , Yuying Hu , Xing Xu , Fangfang Zhao , Yiren Pi , Jian Qian , Fengping Hu , Xiaoming Peng
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Abstract

Recently, the water pollution caused by antibiotics has become an urgent problem to be solved. In this work, we developed a heterogeneous catalyst based on pyrite (i.e.FeS2) via peracetic acid (PAA) activation and further explored the potential efficacy of tetracycline(TC) antibiotics degradation driven by different pH values. The preparation of pyrite under the action of sulfur species in the system solution can exists not only in a variety of forms, but also its general to produce more SO4•- trend. Mechanism analysis showed that the main active species including non-organic radical (R-O•) and •OH as the dominant reactive oxidized species (ROS) in pyrite(FeS2)/PAA process. This results shown that the presence of different forms of sulfur species played a significant role in Fe(II) regeneration with a result of accelerated PAA activation. In addition, the generation of sulfur species with R-Owas proposed as the primary reactive sites for PAA activation in the TC degradation of free radical primary and secondary change in heterogeneous catalyst/PAA reaction systems. DFT theoretical calculations indicate that the CH3COO• prefers electron transfer with sulfur species, which also fully demonstrated the effect by the dual role of sulfur species in regulating the reactive oxidized species and Fe(II) regeneration. Finally, this study expanded the application in hydrophilized fiber via electrospinning technology, and FNC fiber film still could still maintain good catalytic activity of TC in the actual water by FNC/PAA system, verifing that FNC fiber film is suitable for the application of various pollutants and actual wastewater. This work could provide strong support for the use of natural minerals as heterogeneous catalysts for PAA activation and formed FNC fiber film in the practical wastewater treatment applications.

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调节pH条件下黄铁矿活化PAA降解四环素:硫种被忽视的作用
近年来,抗生素引起的水污染已成为一个亟待解决的问题。本研究通过过氧乙酸(PAA)活化制备了一种基于黄铁矿(即fes2)的多相催化剂,并进一步探讨了不同pH值驱动下四环素(TC)抗生素降解的潜在功效。黄铁矿的制备在体系溶液中硫种的作用下不仅能以多种形式存在,而且其一般有产生更多SO4•-的趋势。机理分析表明,黄铁矿(FeS2)/PAA过程中主要活性物质包括非有机自由基(R-O•)和•OH,它们是主要的活性氧(ROS)。结果表明,不同形式的硫的存在对Fe(II)的再生起着重要的作用,从而加速了PAA的活化。此外,在非均相催化剂/PAA反应体系中,在TC降解自由基的过程中,与R-O•生成硫种是PAA活化的主要反应位点。DFT理论计算表明,CH3COO•倾向于与硫种之间的电子转移,这也充分证明了硫种在调节活性氧化态和Fe(II)再生中的双重作用。最后,本研究通过静电纺丝技术扩大了在亲水性纤维中的应用,FNC纤维膜通过FNC/PAA体系在实际水中仍能保持良好的TC催化活性,验证了FNC纤维膜适用于各种污染物和实际废水的应用。本研究为利用天然矿物作为多相催化剂活化PAA并形成FNC纤维膜在废水处理中的实际应用提供了有力的支持。
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来源期刊
Separation and Purification Technology
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.
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