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通过流动式非均相电芬顿工艺,在中性 pH 条件下,高效降解磺胺甲恶唑。双金属 ACF/CC@FeOCl-Cu 复合阴极的简便合成。

Facile synthesis of bimetallic ACF/CC@FeOCl-Cu composite cathode for efficient degradation of sulfamethoxazole at neutral pH by a flow-through heterogeneous electro-Fenton process.

机构信息

Beijing Key Laboratory of Aqueous Typical Pollutants Control and Water Quality Safeguard, School of Environment, Beijing Jiaotong University, China.

Beijing Key Laboratory of Aqueous Typical Pollutants Control and Water Quality Safeguard, School of Environment, Beijing Jiaotong University, China.

出版信息

Chemosphere. 2023 Nov;341:139971. doi: 10.1016/j.chemosphere.2023.139971. Epub 2023 Aug 29.

Abstract

Flow-through heterogeneous electro-Fenton (FHEF) process shows a broad prospect for refractory organic pollutants removal. However, maintaining a long-term service life of higher catalytic cathode is crucial for the development of cathode materials, especially for iron-functionalized cathode operated under harsh conditions. In this study, a novel bimetallic CC@FeOCl-Cu composite was synthesized through one-step calcination, coupled with a series of microstructure characterization methodology, including XRD, SEM-EDS, XPS, and FTIR. The superior catalytic activity of CC@FeOCl-Cu could be ascribed to Fe-Cu synergy and better dispersion of FeOCl nanosheets. With the optimal Cu:Fe ratio of 1:60, the bifunctional ACF/CC@FeOCl-Cu cathode was employed in FHEF process, exhibiting an outstanding performance for sulfamethoxazole (SMX) removal over a wide pH range (3.0-9.0). Comparison of experimental results indicated that the ACF/CC@FeOCl-Cu-FHEF process showed higher performance than ACF/CC@FeOCl-FHEF and homogeneous EF processes. The average SMX removal efficiency was 98% and TOC removal efficiency was more than 57% even after 10 cycles. Radical quenching experiments and electron spin resonance test confirmed that OH was the primary active species. More OH was generated in the ACF/CC@FeOCl-Cu-FHEF process because the doping of Cu could enhance catalytic activity of cathode. In addition, the satisfactory performance could be observed in the ACF/CC@FeOCl-Cu-FHEF process for the treatment of real landfill leachate, indicating its potential for practical application in wastewater treatment.

摘要

流动式多相电芬顿(FHEF)工艺在去除难降解有机污染物方面具有广阔的前景。然而,对于阴极材料的发展来说,保持高催化活性的阴极的长期使用寿命至关重要,尤其是在苛刻条件下运行的铁功能化阴极。在这项研究中,通过一步煅烧法合成了一种新型的双金属 CC@FeOCl-Cu 复合材料,并采用一系列微观结构表征方法,包括 XRD、SEM-EDS、XPS 和 FTIR。CC@FeOCl-Cu 的优异催化活性可归因于 Fe-Cu 协同作用和 FeOCl 纳米片的更好分散。在最佳的 Cu:Fe 比为 1:60 时,将双功能 ACF/CC@FeOCl-Cu 阴极应用于 FHEF 工艺中,在较宽的 pH 范围(3.0-9.0)内对磺胺甲恶唑(SMX)的去除表现出卓越的性能。实验结果的比较表明,与 ACF/CC@FeOCl-FHEF 和均相 EF 工艺相比,ACF/CC@FeOCl-Cu-FHEF 工艺具有更高的性能。即使经过 10 个循环,SMX 的平均去除效率仍为 98%,TOC 的去除效率也超过 57%。自由基猝灭实验和电子自旋共振测试证实,OH 是主要的活性物质。由于掺杂 Cu 可以增强阴极的催化活性,因此在 ACF/CC@FeOCl-Cu-FHEF 过程中会产生更多的 OH。此外,在 ACF/CC@FeOCl-Cu-FHEF 工艺中对实际垃圾渗滤液的处理也表现出令人满意的性能,表明其在废水处理中的实际应用潜力。

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