4.6 Article

Catalytic activation of peroxymonosulfate using MnO2@quasi-MOF for singlet oxygen mediated degradation of organic pollutants in water

Journal

APPLIED CATALYSIS A-GENERAL
Volume 646, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcata.2022.118883

Keywords

Peroxymonosulfate activation efficiency; Quasi-MOF; Metal leaching inhibition; Water remediation; Heterogeneous catalysis

Funding

  1. Cornell Center for Materials Research - NSF MRSEC program [DMR-1719875]
  2. NIH/NIGMS ACERT [P41GM103521]

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Metal organic frameworks (MOFs) are ideal materials for heterogenous catalysis due to their properties such as surface area, porosity, and functionality. In this study, a MnO2@quasi-MOF (MnO2@q-MOF) catalyst was developed by incorporating MnO2 into a MIL-53 (Fe) structure followed by a mild heat treatment. The MnO2@q-MOF catalyst exhibited higher exposed metal sites and activity while preserving the porosity and crystalline structure of MIL-53 (Fe) due to thermally induced decarboxylation and in situ MnO2 formation. The MnO2@q-MOF catalyst was used to activate potassium peroxymonosulfate (PMS) for the decomposition of methylene blue and HEPES in water, showing superior performance compared to MIL-53 (Fe) and unsupported MnO2. The primary mechanism of PMS activation was found to be a singlet oxygen (1O2) mediated process.
The properties of metal organic frameworks (MOFs), surface area, porosity, and functionality make them an ideal material for heterogenous catalysis. We developed a MnO2@quasi-MOF (MnO2@q-MOF) catalyst by incorpo-rating MnO2 into a MIL-53 (Fe) structure with reduction of KMnO4 to MnO2 followed by a mild heat treatment at 300 degrees C. MnO2@q-MOF showed higher exposed metal sites due to thermally induced decarboxylation and higher activity because of in situ MnO2 formation while preserving the porosity and crystalline structure of MIL-53 (Fe). We activated potassium peroxymonosulfate (PMS) using our MnO2@q-MOF catalyst for decomposition of methylene blue and HEPES in water. The MnO2@q-MOF catalyst outperformed both MIL-53 (Fe) and unsup-ported MnO2 in the degradation of dye and was reusable. The primary mechanism of PMS activation was revealed to be a singlet oxygen (1O2) mediated process.

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