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Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation

[Image: see text] Iron- and cobalt-based heterogeneous catalysts are widely applied for activating peroxymonosulfate (PMS) to degrade organic pollutants. However, few studies have unveiled the clear synergistic mechanism of iron and cobalt in ZSM-5. In this paper, the synergistic mechanism of enhanc...

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Autores principales: Yan, Yaqian, Zhang, Xinyi, Wei, Jiahao, Chen, Miao, Bi, Jingtao, Bao, Ying
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9161407/
https://www.ncbi.nlm.nih.gov/pubmed/35664623
http://dx.doi.org/10.1021/acsomega.2c01031
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author Yan, Yaqian
Zhang, Xinyi
Wei, Jiahao
Chen, Miao
Bi, Jingtao
Bao, Ying
author_facet Yan, Yaqian
Zhang, Xinyi
Wei, Jiahao
Chen, Miao
Bi, Jingtao
Bao, Ying
author_sort Yan, Yaqian
collection PubMed
description [Image: see text] Iron- and cobalt-based heterogeneous catalysts are widely applied for activating peroxymonosulfate (PMS) to degrade organic pollutants. However, few studies have unveiled the clear synergistic mechanism of iron and cobalt in ZSM-5. In this paper, the synergistic mechanism of enhanced PMS activation was revealed by constructing iron and cobalt bimetal modified ZSM-5 zeolite catalysts (FeCo-ZSM-5). The tetracycline hydrochloride (TCH) degradation experiments showed that the catalytic activity of FeCo-ZSM-5-2:3 was much higher than those of Fe-ZSM-5 and Co-ZSM-5. In addition, the influences of catalyst dosage, PMS concentration, reaction temperature, initial pH, and coexisting ions on TCH removal were systematically investigated in this paper. Density functional theory calculations indicated that Co was the main active site for PMS adsorption, and Fe increased the area of Co’s positive potential mapped to the electron cloud. The Fe–Co bimetallic doping increased the area of positive potential mapped to the electron cloud and benefited the adsorption of PMS on the catalyst surface, which revealed the synergistic mechanism of bimetals. Electron paramagnetic resonance spectra and quenching experiments showed that sulfate radicals, singlet oxygen, and hydroxyl radicals were involved in the degradation of TCH. Furthermore, liquid chromatography–mass spectrometry was conducted to propose possible degradation pathways. This work provides certain guiding significance in understanding the synergistic effect of heterogeneous catalysts for tetracycline wastewater treatment.
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spelling pubmed-91614072022-06-03 Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation Yan, Yaqian Zhang, Xinyi Wei, Jiahao Chen, Miao Bi, Jingtao Bao, Ying ACS Omega [Image: see text] Iron- and cobalt-based heterogeneous catalysts are widely applied for activating peroxymonosulfate (PMS) to degrade organic pollutants. However, few studies have unveiled the clear synergistic mechanism of iron and cobalt in ZSM-5. In this paper, the synergistic mechanism of enhanced PMS activation was revealed by constructing iron and cobalt bimetal modified ZSM-5 zeolite catalysts (FeCo-ZSM-5). The tetracycline hydrochloride (TCH) degradation experiments showed that the catalytic activity of FeCo-ZSM-5-2:3 was much higher than those of Fe-ZSM-5 and Co-ZSM-5. In addition, the influences of catalyst dosage, PMS concentration, reaction temperature, initial pH, and coexisting ions on TCH removal were systematically investigated in this paper. Density functional theory calculations indicated that Co was the main active site for PMS adsorption, and Fe increased the area of Co’s positive potential mapped to the electron cloud. The Fe–Co bimetallic doping increased the area of positive potential mapped to the electron cloud and benefited the adsorption of PMS on the catalyst surface, which revealed the synergistic mechanism of bimetals. Electron paramagnetic resonance spectra and quenching experiments showed that sulfate radicals, singlet oxygen, and hydroxyl radicals were involved in the degradation of TCH. Furthermore, liquid chromatography–mass spectrometry was conducted to propose possible degradation pathways. This work provides certain guiding significance in understanding the synergistic effect of heterogeneous catalysts for tetracycline wastewater treatment. American Chemical Society 2022-05-17 /pmc/articles/PMC9161407/ /pubmed/35664623 http://dx.doi.org/10.1021/acsomega.2c01031 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Yan, Yaqian
Zhang, Xinyi
Wei, Jiahao
Chen, Miao
Bi, Jingtao
Bao, Ying
Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title_full Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title_fullStr Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title_full_unstemmed Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title_short Understanding the Iron-Cobalt Synergies in ZSM-5: Enhanced Peroxymonosulfate Activation and Organic Pollutant Degradation
title_sort understanding the iron-cobalt synergies in zsm-5: enhanced peroxymonosulfate activation and organic pollutant degradation
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9161407/
https://www.ncbi.nlm.nih.gov/pubmed/35664623
http://dx.doi.org/10.1021/acsomega.2c01031
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