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pH adjustable MgAl@LDH-coated MOFs-derived Co2.25Mn0.75O4 for SMX degradation in PMS activated system
Chenxin Su1, Nizi Zhang1, Xiaobiao Zhu1
1Research Group of Water Pollution Control and Water Reclamation, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, PR China.
Abstract:
Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO4·- was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system.
Insights
A novel core-shell catalyst effectively degrades antibiotic pollution using sulfate radical-based advanced oxidation processes (SR-AOPs). This catalyst shows high efficiency and low toxicity, offering a promising solution for environmental remediation.
Area of Science:
- Environmental Chemistry
- Materials Science
- Catalysis
Background:
- Antibiotic pollution poses a significant environmental threat.
- Sulfate radical-based advanced oxidation processes (SR-AOPs) are effective for pollutant degradation.
- Developing efficient and stable catalysts is crucial for SR-AOPs.
Purpose of the Study:
- To synthesize and evaluate a novel core-shell catalyst for peroxymonosulfate (PMS) activation.
- To degrade sulfamethoxazole (SMX) using the developed catalyst.
- To investigate catalyst stability and degradation pathways.
Main Methods:
- Synthesis of a cobalt-manganese oxide core-shell catalyst (Co/Mn@LDH) derived from CoMn-MOFs and coated with MgAl-LDH.
- Peroxymonosulfate (PMS) activation for SMX degradation.
- Inductively coupled plasma (ICP) for cobalt ion leaching detection.
- Density functional theory (DFT) and liquid chromatography-mass spectrometry (LC-MS) for mechanistic studies.
Main Results:
- Nearly 100% SMX degradation and 68.3% mineralization efficiency achieved.
- The MgAl-LDH shell significantly suppressed cobalt ion leaching (23 μg/L detected).
- Sulfate radical (SO4·-) identified as the dominant reactive species.
- DFT and LC-MS revealed SMX degradation pathways and intermediates with lower toxicity.
Conclusions:
- The Co/Mn@LDH catalyst demonstrates high efficiency and stability for SMX degradation via SR-AOPs.
- The catalyst exhibits excellent performance in activating PMS, with minimal metal leaching.
- The developed catalyst shows significant potential for treating antibiotic pollution in wastewater.
