SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2025, Vol. 80 ›› Issue (4): 248-260.DOI: 10.1016/j.cjche.2024.11.020

Previous Articles     Next Articles

Fe, N-decorated carbocatalyst based on Fe-MOF as PDS activator for efficient sulfadiazine degradation: An electron transfer process

Jiayi Xu1,2, Shuang Li1,2, Wei Zhang1,2,3, Guangli Xiu1,2,3   

  1. 1 State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China;
    2 Shanghai Environmental Protection Key Laboratory on Environmental Standard and Risk Management of Chemical Pollutants, East China University of Science and Technology, Shanghai 200237, China;
    3 Shanghai Institute of Pollution Control and Ecological Security, Tongji University, Shanghai 200092, China
  • Received:2024-06-13 Revised:2024-11-08 Accepted:2024-11-17 Online:2025-01-29 Published:2025-04-28
  • Contact: Wei Zhang,E-mail:zhangwei@ecust.edu.cn
  • Supported by:
    This work is supported by Key Research and Development Projects of Shanghai Municipal Commission of Science and Technology (20dz1204000).

Fe, N-decorated carbocatalyst based on Fe-MOF as PDS activator for efficient sulfadiazine degradation: An electron transfer process

Jiayi Xu1,2, Shuang Li1,2, Wei Zhang1,2,3, Guangli Xiu1,2,3   

  1. 1 State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China;
    2 Shanghai Environmental Protection Key Laboratory on Environmental Standard and Risk Management of Chemical Pollutants, East China University of Science and Technology, Shanghai 200237, China;
    3 Shanghai Institute of Pollution Control and Ecological Security, Tongji University, Shanghai 200092, China
  • 通讯作者: Wei Zhang,E-mail:zhangwei@ecust.edu.cn
  • 基金资助:
    This work is supported by Key Research and Development Projects of Shanghai Municipal Commission of Science and Technology (20dz1204000).

Abstract: In this study, a Fe, N-decorated carbocatalyst (FeCN@X) based on Fe-MOFs was synthesized to activate peroxydisulfate (PDS) for removing sulfadiazine (SDZ) from water. The surface morphology and structure of FeCN@X was characterized by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spec troscopy. FeCN@1000, formed at the pyrolysis temperature of 1000 ℃, exhibited the best catalytic performance for degrade SDZ in the presence of 0.15 g·L-1 catalyst and 0.5 mmol·L-1 PDS, and the reaction conversion rate was 0.199 L·mmol-1. Moreover, the effects of experimental conditions, co-existing anions and fulvic acid on catalytic performance of FeCN@1000 were investigated. The excellent potential of FeCN@1000 as a PDS activator in environmental applications was also suggested by the results of its reusability and adaptability experiments. The result of XPS, ROS quenching, EPR and electrochemical experiments showed the degradation of SDZ was primarily driven by an electron transfer process (ETP). Furthermore, Fe(III) instead of Fe(II) plays a major role in ETP, as Fe(III) sites can interact with PDS and form the low-spin surface complexes (Fe(III)/CN-PDS). Meanwhile, the small number of 1O2 and O2-· generated by the activation of PDS will promote the system degradation of SDZ activity by accelerating the conversion of Fe(II) to Fe(III). This study provides new insights for the design of novel PDS activator for efficient degradation of emerging pollutants by ETP.

Key words: Carbocatalyst, Iron, Peroxydisulfate, Electron transfer, Sulfadiazine

摘要: In this study, a Fe, N-decorated carbocatalyst (FeCN@X) based on Fe-MOFs was synthesized to activate peroxydisulfate (PDS) for removing sulfadiazine (SDZ) from water. The surface morphology and structure of FeCN@X was characterized by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spec troscopy. FeCN@1000, formed at the pyrolysis temperature of 1000 ℃, exhibited the best catalytic performance for degrade SDZ in the presence of 0.15 g·L-1 catalyst and 0.5 mmol·L-1 PDS, and the reaction conversion rate was 0.199 L·mmol-1. Moreover, the effects of experimental conditions, co-existing anions and fulvic acid on catalytic performance of FeCN@1000 were investigated. The excellent potential of FeCN@1000 as a PDS activator in environmental applications was also suggested by the results of its reusability and adaptability experiments. The result of XPS, ROS quenching, EPR and electrochemical experiments showed the degradation of SDZ was primarily driven by an electron transfer process (ETP). Furthermore, Fe(III) instead of Fe(II) plays a major role in ETP, as Fe(III) sites can interact with PDS and form the low-spin surface complexes (Fe(III)/CN-PDS). Meanwhile, the small number of 1O2 and O2-· generated by the activation of PDS will promote the system degradation of SDZ activity by accelerating the conversion of Fe(II) to Fe(III). This study provides new insights for the design of novel PDS activator for efficient degradation of emerging pollutants by ETP.

关键词: Carbocatalyst, Iron, Peroxydisulfate, Electron transfer, Sulfadiazine