Citation: Yu-Ke ZHU, Xiao-Jia JIANG, Jia-Yi CHEN, Xiao-Hang FU, Li-Guang WU, Ting WANG. Mechanism and pathways for degrading tetracycline via photocatalytic synergistic peroxysulfate-activated catalytic oxidation[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(10): 1857-1868. doi: 10.11862/CJIC.2023.164 shu

Mechanism and pathways for degrading tetracycline via photocatalytic synergistic peroxysulfate-activated catalytic oxidation

Yu-Ke ZHU ¹ ,
Xiao-Jia JIANG ^{1, 2} ,
Jia-Yi CHEN ¹ ,
Xiao-Hang FU ¹ ,
Li-Guang WU ¹ ,
Ting WANG ^{1, 2,,}

1.
School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310012, China
2.
Instrumental Analysis Center, Zhejiang Gongshang University, Hangzhou 310012, China

Corresponding author: Ting WANG, zjwtwaiting@hotmail.com
Received Date: 26 May 2023
Revised Date: 22 June 2023

Figures(10)

Aiming at enhancing the degradation efficiency of antibiotics in slightly polluted water bodies, the photocatalytic synergistic sodium peroxysulfate (PDS)-activated catalytic oxidation using chiral mesoporous TiO₂ under irradiation of visible light (PDS/vis-TiO₂) was employed to degrade tetracycline (TC). The differences in active species and degradation pathways of PDS activation (PDS/TiO₂), visible light photocatalysis (vis-TiO₂), and PDS/vis-TiO₂ systems using mesoporous TiO₂ as catalysts for TC degradation were comparatively studied. The results showed that the asymmetric helical stacking structure introduced abundant Ti³⁺ into chiral mesoporous TiO₂, not only improving its visible light response but also activating PDS by Ti³⁺/Ti⁴⁺ couples to form free radicals. Both the photogenerated holes h⁺ and the free radicals (like ·OH) in the PDS/vis-TiO₂ system could simultaneously participate in TC degradation. Within 5 h, the removal rate of TC (the concentration of TC in the solution was 5 mg·L^-1) using the PDS/vis-TiO₂ system could reach over 95%, far exceeding that of the PDS/TiO₂ system (with a TC removal rate of 48.9%) and the vis-TiO₂ system (with a TC removal rate of 71.1%). PDS/vis-TiO₂ system had a high removal rate of TC in solutions with different concentrations, and the degradation all followed a first-order kinetic reaction process. Even when the initial concentration of TC reached 15 mg·L^-1, the 5 h removal rate of TC by PDS/vis-TiO₂ system could still reach 67.2%, which further indicated that the PDS synergistic photocatalysis had an effective ability to degrade TC. However, the removal rate of TC at low concentrations by PDS/vis-TiO₂ was faster than using the same amount of TiO₂ catalyst and PDS. Added PDS in the photocatalytic system would be activated by the photo-generated electrons to generate free radicals, which then consume photo-generated electrons to improve the separation rate of photo-generated holes and electrons, thus achieving synergistic enhancement on the pollutant degradation. Additionally, the free radicals after PDS activation would also enhance TC degradation. The density functional theory calculation and intermediate product analysis results indicate that the degradation pathway of TC in the PDS/vis-TiO₂ system includes the degradation pathway of attacking TC by h⁺, as well as the degradation pathway of TC after the free radicals attack.
- chiral mesoporous TiO₂,
- visible light photocatalysis,
- peroxysulfate activation,
- tetracycline,
- degradation pathway
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