Spatiotemporally optimized dual-stage electro-Fenton system with etched Fe⁰-Fe3O4/CF cathode for efficient sulfadiazine degradation

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Yanshi Zheng, Jinyan Yang, Mei Li, Jiayu Liang, Dehai Yu, Ziyao Wang, Xiao Shan, Gaofeng Pan, Jianchuan Pei
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引用次数: 0

Abstract

Sulfadiazine (SDZ), a potent antibiotic resistant to conventional biological treatment, presents considerable environmental risks if discharged untreated. Electro-Fenton (EF) is a promising technology in SDZ removal. However, oxygen reduction reaction (ORR) performance deterioration caused by iron deposition and the diverse optimal operating conditions for ORR and ferric reduction reaction (FRR) significantly affect the durability and the SDZ removal efficiency in EF system. In this study, a dual-stage spatiotemporal separation heterogeneous EF system was constructed, employing an air-breathing cathode (ABC) in the first stage and a Fe0-Fe3O4/CF cathode in the second stage, which effectively addresses the inherent limitations of EF systems by separating the ORR, H2O2 activation, and FRR spatiotemporally. A novel K2FeO4 etching method was employed to fabricate the Fe0-Fe3O4/CF cathode, ensuring uniformly dispersed active sites within pores. Under optimal operating conditions, the system achieved complete SDZ degradation in 10 min and 80.42 % total organic carbon (TOC) removal. High Fe(II) retention (55.12 %) on Fe0-Fe3O4/CF25 after reaction was observed due to effective FRR. Mechanism studies confirmed that ·OH generated from heterogeneous Fenton dominated SDZ degradation, with DFT analysis confirming electron transfer from SDZ to ·OH. The system demonstrated high durability and low energy consumption, maintaining the ability to completely degrade SDZ in 30 min after six uses, with an energy consumption of 8.48 kWh (kg SDZ)-1 and 0.26 kWh (g TOC)-1. These findings provide ideas for constructing EF systems with higher SDZ removal efficiency and durability.

Abstract Image

具有蚀刻Fe⁰-Fe3O4/CF阴极的时空优化双级电fenton系统,用于有效的磺胺嘧啶降解
磺胺嘧啶(SDZ)是一种对常规生物处理具有耐药性的强效抗生素,如果未经治疗就排放,会带来相当大的环境风险。电fenton (EF)是一种很有前途的SDZ去除技术。然而,铁沉积引起的氧还原反应(ORR)性能下降以及ORR和铁还原反应(FRR)的不同最佳操作条件显著影响了EF系统的耐久性和SDZ去除效率。本研究构建了一种双级时空分离异质EF系统,第一级采用吸气式阴极(ABC),第二级采用Fe0-Fe3O4/CF阴极,有效地解决了EF系统的固有局限性,实现了ORR、H2O2活化和FRR的时空分离。采用一种新颖的K2FeO4刻蚀方法制备Fe0-Fe3O4/CF阴极,保证了孔内活性位点的均匀分散。在最佳操作条件下,系统在10 min内实现了SDZ的完全降解,总有机碳(TOC)去除率为80.42 %。反应后Fe0-Fe3O4/CF25上Fe(II)保留率较高(55.12 %)。机理研究证实,非均相Fenton产生的·OH主导了SDZ的降解,DFT分析证实了SDZ向·OH的电子转移。该系统表现出高耐用性和低能耗,在6次使用后保持在30 min内完全降解SDZ的能力,能耗为8.48 kWh (kg SDZ)-1和0.26 kWh (g TOC)-1。这些发现为构建具有更高SDZ去除效率和耐久性的EF系统提供了思路。
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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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