Mechanism comparison of heterogeneous and electro-enhanced heterogeneous activation of peroxymonosulfate based on CoFe2O4 nanoparticles for gatifloxacin degradation

IF 5.6 3区 材料科学 Q1 ELECTROCHEMISTRY Electrochimica Acta Pub Date : 2025-02-07 DOI:10.1016/j.electacta.2025.145821
Meng Zhang , Tianyi Wang , Guanhong Liu , Rui Zhan , Zhiping Wang , Lili Liu
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Abstract

Mechanisms for gatifloxacin (GAT) degradation had been comparative studied for CoFe2O4 nanoparticles (NPs) based heterogeneous catalytic reaction (HCR) and its electrochemical strengthening method (EC-HCR), as peroxymonosulfate (PMS) was used for oxidant. The results indicated that EC could significantly promote the reaction rate of HCR in 10 mins due to the acceleration of Co/Fe redox cycle and electron transfer between them, and slow down due to the isolation of catalytic active sites by adsorbate since then. Different from the dominant role of SO4•− in HCR system, OH played a pivotal role in EC-HCR system due to the generation of high-valent metal species (HVMS), which also given it greater resistance to the coexisted anions and humic acid. Neither increasing the dosage of CoFe2O4 NPs nor PMS could achieve efficient mineralization of GAT (33.7 % to 41.6 %) in HCR system, while the mineralization efficiencies of GAT were reached 80.4 % and 86.4 % as the mass ratio of PMS to CoFe2O4 were 3:1 and 5:1, respectively. Although the similar GAT degradation pathways were observed in HCR and EC-HCR system attributed to the similar active species composition, the difference in dominant active species caused a very different detoxification effect. The harmful degradation products that presence in HCR system could be degraded in EC-HCR system, with the same CoFe2O4 NPs and PMS dosage. Therefore, EC-HCR can be flexibly applied to the treatment of wastewater that containing antibiotics, either detoxification or complete mineralization depends on the chemical inputs.
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基于CoFe2O4纳米颗粒的过氧单硫酸盐非均相和电增强非均相活化降解加替沙星的机理比较
以过氧单硫酸根(PMS)为氧化剂,比较研究了CoFe2O4纳米颗粒(NPs)非均相催化反应(HCR)及其电化学强化法(EC-HCR)对加替沙星(GAT)的降解机理。结果表明,EC可以显著促进HCR在10 min内的反应速率,这主要是由于Co/Fe氧化还原循环的加速和它们之间的电子转移,而此后由于吸附物分离了催化活性位点而减慢了反应速率。与SO4•−在HCR体系中的主导作用不同,•OH在EC-HCR体系中起着关键作用,因为它产生了高价金属物种(high-valent metal species, HVMS),这也使其对共存的阴离子和腐植酸具有更大的抗性。在HCR体系中,增加CoFe2O4 NPs和PMS的投加量均不能实现GAT的高效矿化(33.7% ~ 41.6%),而PMS与CoFe2O4的质量比分别为3:1和5:1时,GAT的矿化效率分别达到80.4%和86.4%。由于活性种组成相似,HCR和EC-HCR体系的GAT降解途径相似,但优势活性种的差异导致其解毒效果大不相同。在CoFe2O4 NPs和PMS投加量相同的情况下,EC-HCR体系可以降解HCR体系中存在的有害降解产物。因此,EC-HCR可以灵活地应用于含抗生素废水的处理,取决于化学投入,是解毒还是完全矿化。
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来源期刊
Electrochimica Acta
Electrochimica Acta 工程技术-电化学
CiteScore
11.30
自引率
6.10%
发文量
1634
审稿时长
41 days
期刊介绍: Electrochimica Acta is an international journal. It is intended for the publication of both original work and reviews in the field of electrochemistry. Electrochemistry should be interpreted to mean any of the research fields covered by the Divisions of the International Society of Electrochemistry listed below, as well as emerging scientific domains covered by ISE New Topics Committee.
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