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作者:

Wang, Jiong (Wang, Jiong.) | Liu, Zhibin (Liu, Zhibin.) | Sun, Zhirong (Sun, Zhirong.) (学者:孙治荣)

收录:

EI Scopus SCIE

摘要:

In this study, a graphite felt (GF) electrode material supporting a Cu-based catalyst (CuHDC-400/GF) was pre-pared by a hydrothermal process and subsequent heat treatment. A heterogeneous electro-Fenton (EF) system was built to investigate the degradation of sulfamethoxazole (SMX) by the composite cathode. Scanning electron microscopy, X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy were used to char-acterize the physical and chemical properties of the composite cathode. The results show that the composite cathode CuHDC-400/GF has excellent catalytic performance, achieving 100 % removal of SMX (10 mg/L) within 45 min (aeration rate = 0.6 L min(-1), current density = 5 mA cm(-2), initial pH = 5.6). Furthermore, efficient removal of SMX can be achieved over a wide pH range (pH = 3-9). The electrode material can still efficiently degrade SMX after eight cycles. Compared with a heterogeneous EF system, in which the Cu catalyst was directly added to the reaction solution, using CuHDC-400/GF as the cathode realizes the in-situ catalysis of H2O2, leading to reduced catalyst consumption and enhanced electrode stability. The investigation of potential SMX degra-dation pathways and mechanisms revealed that the continuous production of active free radicals is facilitated by the redox cycle between Cu-I and Cu-II on the electrode surface, which can enable SMX degradation. Unlike the Fe-based Fenton reaction, the active superoxide radical O-center dot(2)- was identified as the major contributor to SMX degradation in this system, followed by the hydroxyl radical (OH)-O-center dot. The active sites for SMX degradation were predicted by density functional theory calculations. Combined with the measured mass/charge ratios, the possible degradation paths and intermediates of SMX were predicted. Furthermore, toxicity analysis shows that toxicity significantly declines after degradation. This work is expected to inspire subsequent research on het-erogeneous EF cathode materials with high catalytic performance.

关键词:

Metal-organic framework Heterogeneous electro-Fenton Sulfamethoxazole Degradation mechanism In-situ catalysis

作者机构:

  • [ 1 ] [Sun, Zhirong]Beijing Univ Technol, Fac Environm & Life, Dept Environm Engn, Beijing 100124, Peoples R China
  • [ 2 ] [Sun, Zhirong]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Beijing 100124, Peoples R China

通讯作者信息:

  • [Sun, Zhirong]Beijing Univ Technol, Fac Environm & Life, Dept Environm Engn, Beijing 100124, Peoples R China;;

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来源 :

SEPARATION AND PURIFICATION TECHNOLOGY

ISSN: 1383-5866

年份: 2023

卷: 316

8 . 6 0 0

JCR@2022

ESI学科: CHEMISTRY;

ESI高被引阀值:20

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