4.7 Article

Constructing a 3D interconnected trap-zap β-CDPs/Fe-g-C3N4 catalyst for efficient sulfamethoxazole degradation via peroxymonosulfate activation: Performance, mechanism, intermediates and toxicity

Journal

CHEMOSPHERE
Volume 294, Issue -, Pages -

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2022.133780

Keywords

Peroxymonosulfate; Cyclodextrin polymer; Fe-g-C3N4; Sulfamethoxazole

Funding

  1. National Natural Science Foundation of China [22166016, 21866012]
  2. Hainan Provincial Key Research and Development Program [ZDYF2020222]
  3. Graduate Innovation Research Project of Hainan [Hys 2020-183]
  4. Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province [AFEPER202101]
  5. Hainan Provincial Natural Science Foundation [521QN210]
  6. Youth Fund Project of Hainan University [HDQN202113]

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A novel Fe-doped g-C3N4 catalyst composited with beta-cyclodextrin polymers (beta-CDPs) was synthesized for peroxymonosulfate (PMS) activation. The catalyst exhibited a 3D interconnected porous structure and showed superior degradation performance in a wide pH range with good selectivity. The main active species for PMS activation were identified to be Fe(V)--O and O-1(2) based on radical scavenging, EPR, and electrochemical measurements.
A novel and high-efficiency catalyst Fe doped g-C3N4 (Fe-g-C3N4) composited with beta-cyclodextrin polymers (beta-CDPs) was synthesized for activating peroxymonosulfate (PMS). The scanning electron microscopy (SEM) and transmission electron microscopy (TEM) results showed that the catalyst was 3D interconnected porous structure. The degradation rate constant of sulfamethoxazole (SMX) in beta-CDPs/Fe-g-C3N4+PMS system was estimated to be 0.132 min (-1), which was 14.7 times and 2.2 times that of g-C3N4+PMS and Fe-g-C3N4+PMS system, respectively. In addition, the beta-CDPs/Fe-g-C3N4 exhibited superior degradation performance in a wide pH range (3.0-9.0) and good selectivity in the presence of other inorganic anions and natural organics. Radical scavenging, electron paramagnetic resonance (EPR) and electrochemical measurements indicated that O-1(2) and Fe(V)--O were the main active species for SMX degradation in beta-CDPs/Fe-g-C3N4+PMS system. Moreover, beta-CDPs accelerated electron transfer between catalyst and PMS and promoted the generation of reactive oxygen species (ROS) during PMS activation. The loading of beta-CDPs increased the yields of Fe(V)--O and O-1(2) in the system and limited the leaching of Fe3+. In addition, the possible degradation pathways of SMX were described based on the intermediates detected by liquid chromatography-mass spectrometry (LC-MS), and the toxicity of the intermediates was also evaluated. This work investigate the role of 8-CDPs in PMS activation for the first time and develop a promising material with potential for water treatment.

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