Activation performance and mechanism of a novel heterogeneous persulfate catalyst: Metal-organic framework MIL-53(Fe) with FeII/FeIII mixed-valence coordinatively unsaturated iron center

Mengjie Pu, Yongwen Ma, Jinquan Wan, Yan Wang, Jiumei Wang, Mark L. Brusseau

Research output: Research - peer-reviewArticle

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Abstract

In this work, a novel and effective heterogeneous catalyst, the metal-organic framework MIL-53(Fe), has been synthesized for the purpose of activating persulfate (PS). The catalytic performance of MIL-53(Fe) activated under different vacuum conditions was investigated; the stability and reusability of the catalyst were evaluated, and the activation mechanism was also investigated. The results indicated that vacuum activation could cause variation of the FeII/FeIII relative amount ratio of the catalyst, and thus would change the catalytic activity of MIL-53(Fe), because FeII and FeIII CUS (coordinatively unsaturated metal sites) are alternative active sites. It was found that MIL-53(Fe)-2 exhibits good performance in PS activation and could be used for multiple cycles; an OG removal rate of 98% was obtained within 120 min (95.7% mineralization efficiency) and 94.3% was achieved in the fifth cycle. The mechanism of activation of PS by MIL-53(Fe) was also suggested, which involved a predominant heterogeneous reaction and an auxiliary homogeneous reaction. The findings of this study provide a new insight into the application of reactive metal-organic frameworks in activating persulfate for the degradation of environmental contaminants.

LanguageEnglish (US)
Pages1129-1140
Number of pages12
JournalCatalysis Science and Technology
Volume7
Issue number5
DOIs
StatePublished - 2017

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Iron
Metals
Chemical activation
Catalysts
N(1)-methyl-2-lysergic acid diethylamide
Vacuum
Reusability
Catalyst activity
Impurities
Degradation

ASJC Scopus subject areas

  • Catalysis

Cite this

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title = "Activation performance and mechanism of a novel heterogeneous persulfate catalyst: Metal-organic framework MIL-53(Fe) with FeII/FeIII mixed-valence coordinatively unsaturated iron center",
abstract = "In this work, a novel and effective heterogeneous catalyst, the metal-organic framework MIL-53(Fe), has been synthesized for the purpose of activating persulfate (PS). The catalytic performance of MIL-53(Fe) activated under different vacuum conditions was investigated; the stability and reusability of the catalyst were evaluated, and the activation mechanism was also investigated. The results indicated that vacuum activation could cause variation of the FeII/FeIII relative amount ratio of the catalyst, and thus would change the catalytic activity of MIL-53(Fe), because FeII and FeIII CUS (coordinatively unsaturated metal sites) are alternative active sites. It was found that MIL-53(Fe)-2 exhibits good performance in PS activation and could be used for multiple cycles; an OG removal rate of 98% was obtained within 120 min (95.7% mineralization efficiency) and 94.3% was achieved in the fifth cycle. The mechanism of activation of PS by MIL-53(Fe) was also suggested, which involved a predominant heterogeneous reaction and an auxiliary homogeneous reaction. The findings of this study provide a new insight into the application of reactive metal-organic frameworks in activating persulfate for the degradation of environmental contaminants.",
author = "Mengjie Pu and Yongwen Ma and Jinquan Wan and Yan Wang and Jiumei Wang and Brusseau, {Mark L.}",
year = "2017",
doi = "10.1039/c6cy02355j",
volume = "7",
pages = "1129--1140",
journal = "Catalysis Science and Technology",
issn = "2044-4753",
publisher = "Royal Society of Chemistry",
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TY - JOUR

T1 - Activation performance and mechanism of a novel heterogeneous persulfate catalyst

T2 - Catalysis Science and Technology

AU - Pu,Mengjie

AU - Ma,Yongwen

AU - Wan,Jinquan

AU - Wang,Yan

AU - Wang,Jiumei

AU - Brusseau,Mark L.

PY - 2017

Y1 - 2017

N2 - In this work, a novel and effective heterogeneous catalyst, the metal-organic framework MIL-53(Fe), has been synthesized for the purpose of activating persulfate (PS). The catalytic performance of MIL-53(Fe) activated under different vacuum conditions was investigated; the stability and reusability of the catalyst were evaluated, and the activation mechanism was also investigated. The results indicated that vacuum activation could cause variation of the FeII/FeIII relative amount ratio of the catalyst, and thus would change the catalytic activity of MIL-53(Fe), because FeII and FeIII CUS (coordinatively unsaturated metal sites) are alternative active sites. It was found that MIL-53(Fe)-2 exhibits good performance in PS activation and could be used for multiple cycles; an OG removal rate of 98% was obtained within 120 min (95.7% mineralization efficiency) and 94.3% was achieved in the fifth cycle. The mechanism of activation of PS by MIL-53(Fe) was also suggested, which involved a predominant heterogeneous reaction and an auxiliary homogeneous reaction. The findings of this study provide a new insight into the application of reactive metal-organic frameworks in activating persulfate for the degradation of environmental contaminants.

AB - In this work, a novel and effective heterogeneous catalyst, the metal-organic framework MIL-53(Fe), has been synthesized for the purpose of activating persulfate (PS). The catalytic performance of MIL-53(Fe) activated under different vacuum conditions was investigated; the stability and reusability of the catalyst were evaluated, and the activation mechanism was also investigated. The results indicated that vacuum activation could cause variation of the FeII/FeIII relative amount ratio of the catalyst, and thus would change the catalytic activity of MIL-53(Fe), because FeII and FeIII CUS (coordinatively unsaturated metal sites) are alternative active sites. It was found that MIL-53(Fe)-2 exhibits good performance in PS activation and could be used for multiple cycles; an OG removal rate of 98% was obtained within 120 min (95.7% mineralization efficiency) and 94.3% was achieved in the fifth cycle. The mechanism of activation of PS by MIL-53(Fe) was also suggested, which involved a predominant heterogeneous reaction and an auxiliary homogeneous reaction. The findings of this study provide a new insight into the application of reactive metal-organic frameworks in activating persulfate for the degradation of environmental contaminants.

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