Iron-based metal-organic framework derived pyrolytic materials for effective Fenton-like catalysis: Performance, mechanisms and practicability

In this study, a new catalyst was fabricated by pyrolysis under nitrogen atmosphere with MIL-53(Fe) as the precursor, and was applied to catalyze Fenton-like process. Effects of calcination temperature and pH on decontamination performance, and stability of materials were investigated. Under optimal...

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Veröffentlicht in:The Science of the total environment 2022-02, Vol.809, p.152201-152201, Article 152201
Hauptverfasser: Ren, Yi, Zhang, Jing, Ji, Chenghan, Wang, Shu, Lv, Lu, Zhang, Weiming
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creator Ren, Yi
Zhang, Jing
Ji, Chenghan
Wang, Shu
Lv, Lu
Zhang, Weiming
description In this study, a new catalyst was fabricated by pyrolysis under nitrogen atmosphere with MIL-53(Fe) as the precursor, and was applied to catalyze Fenton-like process. Effects of calcination temperature and pH on decontamination performance, and stability of materials were investigated. Under optimal conditions (calcination temperature of 500 °C and pH of 5.0), the new Fenton-like system remained low iron leaching, and achieved high pseudo-first-order rate constant of 0.0251 min−1 for bisphenol S (BPS) removal, which is much higher than those in MIL-53(Fe), and nano-Fe3O4 catalyzed Fenton-like systems. The superiority of the new catalyst for Fenton-like catalysis was attributed to high specific surface area, as well as formed Fe(II), coordinatively unsaturated iron center and the Fe-O/Fe-C compounds based on the analyses of characterizations. Furthermore, main active species for BPS degradation was identified as hydroxyl radicals, and total hydroxyl radical generation was determined by trapping experiments. The degradation pathways of BPS were also proposed by intermediates monitoring. Moreover, this catalyst showed good potential for practical application, according to the evaluation of reuse, different pollutants degradation, and BPS removal in real wastewater. We believe this study developed a new catalyst with high catalytic activity, high stability and wide application scope, and also sheds light on further development of metal-organic frameworks for Fenton-like catalysis. [Display omitted] •A catalyst was fabricated by pyrolyzing MIL-53(Fe) under nitrogen atmosphere.•The new system exhibited much better bisphenol S removal than control systems.•High specific surface aera and new Fe species formation contributed to high activity.•Superiority remained with different pollutants, real wastewater and for 5 cycles use.
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Effects of calcination temperature and pH on decontamination performance, and stability of materials were investigated. Under optimal conditions (calcination temperature of 500 °C and pH of 5.0), the new Fenton-like system remained low iron leaching, and achieved high pseudo-first-order rate constant of 0.0251 min−1 for bisphenol S (BPS) removal, which is much higher than those in MIL-53(Fe), and nano-Fe3O4 catalyzed Fenton-like systems. The superiority of the new catalyst for Fenton-like catalysis was attributed to high specific surface area, as well as formed Fe(II), coordinatively unsaturated iron center and the Fe-O/Fe-C compounds based on the analyses of characterizations. Furthermore, main active species for BPS degradation was identified as hydroxyl radicals, and total hydroxyl radical generation was determined by trapping experiments. The degradation pathways of BPS were also proposed by intermediates monitoring. Moreover, this catalyst showed good potential for practical application, according to the evaluation of reuse, different pollutants degradation, and BPS removal in real wastewater. We believe this study developed a new catalyst with high catalytic activity, high stability and wide application scope, and also sheds light on further development of metal-organic frameworks for Fenton-like catalysis. [Display omitted] •A catalyst was fabricated by pyrolyzing MIL-53(Fe) under nitrogen atmosphere.•The new system exhibited much better bisphenol S removal than control systems.•High specific surface aera and new Fe species formation contributed to high activity.•Superiority remained with different pollutants, real wastewater and for 5 cycles use.</description><identifier>ISSN: 0048-9697</identifier><identifier>EISSN: 1879-1026</identifier><identifier>DOI: 10.1016/j.scitotenv.2021.152201</identifier><identifier>PMID: 34890672</identifier><language>eng</language><publisher>Netherlands: Elsevier B.V</publisher><subject>Catalysis ; Catalytic mechanisms ; Fenton-like oxidation ; Hydrogen Peroxide ; Iron ; Metal-Organic Frameworks ; Oxidation-Reduction ; Practicability ; Pyrolysis</subject><ispartof>The Science of the total environment, 2022-02, Vol.809, p.152201-152201, Article 152201</ispartof><rights>2021 Elsevier B.V.</rights><rights>Copyright © 2021 Elsevier B.V. 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Moreover, this catalyst showed good potential for practical application, according to the evaluation of reuse, different pollutants degradation, and BPS removal in real wastewater. We believe this study developed a new catalyst with high catalytic activity, high stability and wide application scope, and also sheds light on further development of metal-organic frameworks for Fenton-like catalysis. [Display omitted] •A catalyst was fabricated by pyrolyzing MIL-53(Fe) under nitrogen atmosphere.•The new system exhibited much better bisphenol S removal than control systems.•High specific surface aera and new Fe species formation contributed to high activity.•Superiority remained with different pollutants, real wastewater and for 5 cycles use.</abstract><cop>Netherlands</cop><pub>Elsevier B.V</pub><pmid>34890672</pmid><doi>10.1016/j.scitotenv.2021.152201</doi><tpages>1</tpages></addata></record>
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subjects Catalysis
Catalytic mechanisms
Fenton-like oxidation
Hydrogen Peroxide
Iron
Metal-Organic Frameworks
Oxidation-Reduction
Practicability
Pyrolysis
title Iron-based metal-organic framework derived pyrolytic materials for effective Fenton-like catalysis: Performance, mechanisms and practicability
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