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Published on: September 5, 2018
Densely Stacked CoCu-MOFs Coated with CuAl/LDH Enhance Sulfamethoxazole Degradation in PMS-Activated Systems
Xin Zhong1, Xiaojun Liu2, Meihuan Ji1
1Experimental Education Platform, Beijing Normal University at Zhuhai, Zhuhai 519087, China.
Abstract:
As the most promising techniques for refractory antibiotic degradation in wastewater management, sulfate radical-based advanced oxidation processes (SR-AOPs) have attracted considerable attention. However, systematic studies on potassium peroxymonosulfate (PMS) activation by MOF-derived metal oxides coated with LDH materials are still lacking. In this work, a series of catalysts consisting of CoCu-MOFs coated with CuAl/LDH were synthesized for PMS activation in the removal of sulfamethoxazole (SMX). As expected, CoCu-MOFs coated with CuAl/LDH catalyst showed high SMX removal and stability in PMS activation. In the CoCu/LDH/PMS reaction, the SMX removal was nearly 100% after 60 min, and the mineralization reached 53.7%. The catalyst showed excellent catalytic stability and low metal leaching concentrations (Co: 0.013 mg/L, Cu: 0.313 mg/L), as detected by ICP. Sulfate radicals and hydroxyl radicals were identified as the dominant reactive species in the CoCu/LDH/PMS system. Moreover, the presence of 1O2 in the process revealed the coupling of non-radical and radical processes. The XPS results showed that the layered structure of CoCu/LDH promoted the recycling of metal ions (high and low valence), which facilitated heterogeneous PMS activation. The effects of different reaction conditions and reuse cycles were also determined. The SMX oxidation pathways were proposed based on the intermediates identified by LC/MS. The high activity and stability of CoCu/LDH provide a new mechanistic understanding of PMS activation catalysts and their potential utilization in practical wastewater treatment.
Insights
This study developed a novel catalyst for advanced oxidation processes, effectively degrading refractory antibiotics like sulfamethoxazole (SMX) using potassium peroxymonosulfate (PMS) activation for cleaner wastewater management.
Area of Science:
- Environmental Chemistry
- Materials Science
Background:
- Sulfate radical-based advanced oxidation processes (SR-AOPs) are promising for refractory antibiotic degradation in wastewater.
- Systematic studies on potassium peroxymonosulfate (PMS) activation by MOF-derived metal oxides coated with layered double hydroxide (LDH) materials are limited.
Purpose of the Study:
- To synthesize and evaluate CoCu-MOFs coated with CuAl/LDH as catalysts for PMS activation.
- To investigate the removal efficiency and stability of the catalyst in degrading sulfamethoxazole (SMX).
- To elucidate the reaction mechanism and identify reactive species involved in SMX degradation.
Main Methods:
- Synthesis of CoCu-MOFs coated with CuAl/LDH.
- PMS activation for SMX degradation.
- Analysis of catalyst stability and metal leaching using ICP.
- Identification of reactive species (sulfate radicals, hydroxyl radicals, 1O2) and intermediates (LC/MS).
- XPS analysis to understand the catalyst's electronic structure and metal ion cycling.
Main Results:
- The CoCu/LDH catalyst achieved nearly 100% SMX removal and 53.7% mineralization within 60 minutes.
- The catalyst exhibited excellent stability with low metal leaching (Co: 0.013 mg/L, Cu: 0.313 mg/L).
- Sulfate radicals, hydroxyl radicals, and 1O2 were identified as key reactive species, indicating coupled radical and non-radical pathways.
Conclusions:
- The CoCu/LDH catalyst demonstrates high efficiency and stability for PMS activation in SMX removal.
- The layered structure facilitates metal ion cycling, promoting heterogeneous PMS activation.
- This work provides mechanistic insights into PMS activation catalysts for practical wastewater treatment applications.
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