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Issue 5, 2017
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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

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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.

Graphical abstract: 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

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Publication details

The article was received on 09 Nov 2016, accepted on 28 Jan 2017 and first published on 16 Feb 2017


Article type: Paper
DOI: 10.1039/C6CY02355J
Citation: Catal. Sci. Technol., 2017,7, 1129-1140
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    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

    M. Pu, Y. Ma, J. Wan, Y. Wang, J. Wang and M. L. Brusseau, Catal. Sci. Technol., 2017, 7, 1129
    DOI: 10.1039/C6CY02355J

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