Unveiling the Efficacy and Mechanism of Chlortetracycline Degradation by MnFeCu-LDH/GO Activating of Peroxymonosulfate

Overview

Journal RSC Adv

Publisher Royal Society of Chemistry

Specialty Chemistry

Date 2025 Feb 18

PMID 39963450

Authors

Dongfeng Shi

Xiyin Mao

Min Fei

Cong Liang

Yuyang Luo

Zhidan Xu

Liyong Hu

Affiliations

Soon will be listed here.

Abstract

Antibiotics are frequently detected in aquatic environments, posing potential risks to ecological systems and human health. Among the various treatment strategies, advanced oxidation processes (AOPs) utilizing peroxymonosulfate (PMS) activation stand out due to their ease of activation and potent oxidative capabilities. This study synthesized manganese-iron-copper layered double hydroxides coupled with graphene oxide (MnFeCu-LDH/GO) using eco-friendly transition metals. Optimal conditions of pH 7, 298 K, and 0.2 g L dosage of both catalyst and PMS achieved 98% CTC removal in 30 minutes. The composite was employed for the degradation of chlortetracycline (CTC) through PMS activation. Reactive oxygen species (ROS), including O, ˙OH, and SO˙, were identified and quantified through trapping and quenching experiments, and O was identified, to be the most significant contributor to degradation. The catalyst demonstrated excellent reusability, maintaining high degradation efficiency after five cycles. These findings suggest that MnFeCu-LDH/GO-activated PMS is a promising method for mitigating antibiotic contamination in water.

References

Yuan R, Hu L, Yu P, Wang H, Wang Z, Fang J . Nanostructured CoO grown on nickel foam: An efficient and readily recyclable 3D catalyst for heterogeneous peroxymonosulfate activation. Chemosphere. 2018; 198:204-215. DOI: 10.1016/j.chemosphere.2018.01.135. View

Miklos D, Remy C, Jekel M, Linden K, Drewes J, Hubner U . Evaluation of advanced oxidation processes for water and wastewater treatment - A critical review. Water Res. 2018; 139:118-131. DOI: 10.1016/j.watres.2018.03.042. View

Liu J, Yang Q, Wang D, Li X, Zhong Y, Li X . Enhanced dewaterability of waste activated sludge by Fe(II)-activated peroxymonosulfate oxidation. Bioresour Technol. 2016; 206:134-140. DOI: 10.1016/j.biortech.2016.01.088. View

Tian Y, Feng L, Li R, Li J, Du Z, Zhang L . Inhibitory effects of antioxidant moieties in humic substances on phototransformation of chlortetracycline mediated by the algae extracellular organic matter. Sci Total Environ. 2021; 798:149001. DOI: 10.1016/j.scitotenv.2021.149001. View

Xu Y, Ai J, Zhang H . The mechanism of degradation of bisphenol A using the magnetically separable CuFe2O4/peroxymonosulfate heterogeneous oxidation process. J Hazard Mater. 2016; 309:87-96. DOI: 10.1016/j.jhazmat.2016.01.023. View

Doughty T, Zingl A, Wunschek M, Pichler C, Watkins M, Roy S . Structural Reconstruction of a Cobalt- and Ferrocene-Based Metal-Organic Framework during the Electrochemical Oxygen Evolution Reaction. ACS Appl Mater Interfaces. 2024; 16(31):40814-40824. PMC: 11310903. DOI: 10.1021/acsami.4c03262. View

Yuan Y, Garg S, Ma J, Waite T . Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu-Al Layered Double Hydroxides and Copper Oxide Catalysts. Environ Sci Technol. 2021; 55(19):13274-13285. DOI: 10.1021/acs.est.1c03718. View

Wang L, Jiang N, Xu H, Luo Y, Zhang T . Trace Cu(II)-Mediated Selective Oxidation of Benzothiazole: The Predominance of Sequential Cu(II)-Cu(I)-Cu(III) Valence Transition and Dissolved Oxygen. Environ Sci Technol. 2023; 57(33):12523-12533. DOI: 10.1021/acs.est.3c04134. View

Hou L, Li X, Yang Q, Chen F, Wang S, Ma Y . Heterogeneous activation of peroxymonosulfate using Mn-Fe layered double hydroxide: Performance and mechanism for organic pollutant degradation. Sci Total Environ. 2019; 663:453-464. DOI: 10.1016/j.scitotenv.2019.01.190. View

10.

Zhou L, Li J, Zhang Y, Kong L, Jin M, Yang X . Trends in the occurrence and risk assessment of antibiotics in shallow lakes in the lower-middle reaches of the Yangtze River basin, China. Ecotoxicol Environ Saf. 2019; 183:109511. DOI: 10.1016/j.ecoenv.2019.109511. View

11.

Guo R, Zhu Y, Cheng X, Li J, Crittenden J . Efficient degradation of lomefloxacin by Co-Cu-LDH activating peroxymonosulfate process: Optimization, dynamics, degradation pathway and mechanism. J Hazard Mater. 2020; 399:122966. DOI: 10.1016/j.jhazmat.2020.122966. View

12.

Ben W, Zhu B, Yuan X, Zhang Y, Yang M, Qiang Z . Occurrence, removal and risk of organic micropollutants in wastewater treatment plants across China: Comparison of wastewater treatment processes. Water Res. 2017; 130:38-46. DOI: 10.1016/j.watres.2017.11.057. View

13.

Liu X, Guo X, Liu Y, Lu S, Xi B, Zhang J . A review on removing antibiotics and antibiotic resistance genes from wastewater by constructed wetlands: Performance and microbial response. Environ Pollut. 2019; 254(Pt A):112996. DOI: 10.1016/j.envpol.2019.112996. View

14.

Liu X, Lu S, Guo W, Xi B, Wang W . Antibiotics in the aquatic environments: A review of lakes, China. Sci Total Environ. 2019; 627:1195-1208. DOI: 10.1016/j.scitotenv.2018.01.271. View

15.

Huang G, Wang C, Yang C, Guo P, Yu H . Degradation of Bisphenol A by Peroxymonosulfate Catalytically Activated with MnFeO Nanospheres: Synergism between Mn and Fe. Environ Sci Technol. 2017; 51(21):12611-12618. DOI: 10.1021/acs.est.7b03007. View

16.

Zhao X, Niu C, Zhang L, Guo H, Wen X, Liang C . Co-Mn layered double hydroxide as an effective heterogeneous catalyst for degradation of organic dyes by activation of peroxymonosulfate. Chemosphere. 2018; 204:11-21. DOI: 10.1016/j.chemosphere.2018.04.023. View

17.

Hang Pham T, Rossi P, Khoa Dinh H, Pham N, Tran P, Ho T . Analysis of antibiotic multi-resistant bacteria and resistance genes in the effluent of an intensive shrimp farm (Long An, Vietnam). J Environ Manage. 2018; 214:149-156. DOI: 10.1016/j.jenvman.2018.02.089. View

18.

Fan X, Cao Q, Meng F, Song B, Bai Z, Zhao Y . A Fenton-like system of biochar loading Fe-Al layered double hydroxides (FeAl-LDH@BC) / HO for phenol removal. Chemosphere. 2020; 266:128992. DOI: 10.1016/j.chemosphere.2020.128992. View

19.

Zeng H, Zhang W, Deng L, Luo J, Zhou S, Liu X . Degradation of dyes by peroxymonosulfate activated by ternary CoFeNi-layered double hydroxide: Catalytic performance, mechanism and kinetic modeling. J Colloid Interface Sci. 2018; 515:92-100. DOI: 10.1016/j.jcis.2018.01.016. View

20.

Li Z, Sun Y, Huang W, Xue C, Zhu Y, Wang Q . Innovatively employing magnetic CuO nanosheet to activate peroxymonosulfate for the treatment of high-salinity organic wastewater. J Environ Sci (China). 2019; 88:46-58. DOI: 10.1016/j.jes.2019.07.011. View