Degradation of Bisphenol A by Peroxymonosulfate Catalytically Activated with Mn1.8Fe1.2O4 Nanospheres: Synergism between Mn and Fe

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CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science & Technology of China, Hefei, 230026, China
**. Prof. Han-Qing Yu, Fax: +86 551 63601592; E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2017, 51, 21, 12611–12618
Publication Date (Web):October 6, 2017
https://doi.org/10.1021/acs.est.7b03007
Copyright © 2017 American Chemical Society
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Abstract

A high-efficient, low-cost, and eco-friendly catalyst is highly desired to activate peroxides for environmental remediation. Due to the potential synergistic effect between bimetallic oxides’ two different metal cations, these oxides exhibit superior performance in the catalytic activation of peroxymonosulfate (PMS). In this work, novel Mn1.8Fe1.2O4 nanospheres were synthesized and used to activate PMS for the degradation of bisphenol A (BPA), a typical refractory pollutant. The catalytic performance of the Mn1.8Fe1.2O4 nanospheres was substantially greater than that of the Mn/Fe monometallic oxides and remained efficient in a wide pH range from 4 to 10. More importantly, a synergistic effect between solid-state Mn and Fe was identified in control experiments with Mn3O4 and Fe3O4. Mn was inferred to be the primary active site in the surface of the Mn1.8Fe1.2O4 nanospheres, while Fe(III) was found to play a key role in the synergism with Mn by acting as the main adsorption site for the reaction substrates. Both sulfate and hydroxyl radicals were generated in the PMS activation process. The intermediates of BPA degradation were identified and the degradation pathways were proposed. This work is expected to help to elucidate the rational design and efficient synthesis of bimetallic materials for PMS activation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b03007.

  • The N2 adsorption–desorption isotherms (Figure S1), the XRD patterns (Figure S2), the change of solution pH during the reaction without any buffers (Figure S3) and with 20 mM borate buffer (Figure S4), the effect of borate on BPA degradation (Figure S5), the specific-surface-area normalized catalytic efficiencies (Figure S6) of the catalysts, the BPA removal efficiencies in homogeneous systems (Figure S7) and in repeated batch catalytic reactions (Figure S9), the TOC removal efficiency (Figure S8), the Raman (Figure S10) and FTIR (Figure S11) spectra of the MnFeO samples, the SEM images of Mn3O4/Fe3O4 (Figure S12), the EPR spectra in the presence of EtOH (Figure S13), the XPS spectra of Mn 2p and Fe 2p (Figure S14), the GC-MS chromatogram (Figure S15) and MS spectra (Figure S16) of the intermediates, the proposed pathways (Figure S17) for BPA degradation, the comparison between MnFeO and the previously reported Mn/Fe-oxide catalysts in the catalytic Performance (Table S1), and concentrations of the leaching metal ions after the reaction under various conditions (Table S2) (PDF)

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