Citation: Zhi-Ling Li, Di Cao, Hao Cheng, Fan Chen, Jun Nan, Bin Liang, Kai Sun, Cong Huang, Ai-Jie Wang. Ordered mesoporous carbon as an efficient heterogeneous catalyst to activate peroxydisulfate for degradation of sulfadiazine[J]. Chinese Chemical Letters, ;2022, 33(5): 2747-2752. doi: 10.1016/j.cclet.2021.10.086 shu

Ordered mesoporous carbon as an efficient heterogeneous catalyst to activate peroxydisulfate for degradation of sulfadiazine

Zhi-Ling Li ^a ,
Di Cao ^a ,
Hao Cheng ^a ,
Fan Chen ^{a, c} ,
Jun Nan ^a ,
Bin Liang ^b ,
Kai Sun ^{d, *,} ,
Cong Huang ^e ,
Ai-Jie Wang ^{a, b, *,}

a.
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
b.
School of Civil & Environmental Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
c.
School of Ecology and Environment, Northwestern Polytechnical University, Xi'an 710129, China
d.
Key Lab of Structures Dynamic Behavior and Control of China Ministry of Education, School of Civil Engineering, Harbin Institute of Technology, Harbin 150090, China
e.
National Technology Innovation Center of Synthetic Biology, Tianjin Institute of Industrial Biotechnology, Chinese Academy of Sciences, Tianjin 300308, China

sunkai@hit.edu.cn

waj0578@hit.edu.cn

Received Date: 21 August 2021
Revised Date: 25 September 2021
Accepted Date: 27 October 2021
Available Online: 2 November 2021

Figures(5)

Catalytic potential of carbon nanomaterials in peroxydisulfate (PDS) advanced oxidation systems for degradation of antibiotics remains poorly understood. This study revealed ordered mesoporous carbon (type CMK) acted as a superior catalyst for heterogeneous degradation of sulfadiazine (SDZ) in PDS system, with a first-order reaction kinetic constant (k) and total organic carbon (TOC) mineralization efficiency of 0.06 min^-1 and 59.67% ± 3.4% within 60 min, respectively. CMK catalyzed PDS system exhibited high degradation efficiencies of five other sulfonamides and three other types of antibiotics, verifying the broad-degradation capacity of antibiotics. Under neutral pH conditions, the optimal catalytic parameters were an initial SDZ concentration of 44.0 mg/L, CMK dosage of 0.07 g/L, and PDS dosage of 5.44 mmol/L, respectively. X-ray photoelectron spectroscopy and Raman spectrum analysis confirmed that the defect structure at edge of CMK and oxygen-containing functional groups on surface of CMK were major active sites, contributing to the high catalytic activity. Free radical quenching analysis revealed that both SO₄^·- and ^·OH were generated and participated in catalytic reaction. In addition, direct electron transfer by CMK to activate PDS also occurred, further promoting catalytic performance. Configuration of SDZ molecule was optimized using density functional theory, and the possible reaction sites in SDZ molecule were calculated using Fukui function. Combining ultra-high-performance liquid chromatography (UPLC)–mass spectrometry (MS)/MS analysis, three potential degradation pathways were proposed, including the direct removal of SO₂ molecules, the 14S-17 N fracture, and the 19C-20 N and 19C-27 N cleavage of the SDZ molecule. The study demonstrated that ordered mesoporous carbon could work as a feasible catalytic material for PDS advanced oxidation during removal of antibiotics from wastewater.
- Ordered mesoporous carbon CMK,
- Sulfadiazine,
- Peroxydisulfate,
- Degradation pathway,
- Density functional theory,
- Physicochemical properties
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