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Mixed Conducting Perovskite Materials as Superior Catalysts for Fast Aqueous-Phase Advanced Oxidation: A Mechanistic Study

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Department of Chemical Engineering, Curtin University, Perth, WA 6845, Australia
Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, No. 5 Xin Mofan Road, Nanjing 210009, P. R. China
Cite this: ACS Catal. 2017, 7, 1, 388–397
Publication Date (Web):November 29, 2016
https://doi.org/10.1021/acscatal.6b02303
Copyright © 2016 American Chemical Society
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Abstract

A mixed ionic–electronic conducting (MIEC) double perovskite, PrBaCo2O5+δ (PBC), was synthesized and evaluated as the heterogeneous catalyst to generate radicals from peroxymonosulfate (PMS) for the oxidative degradation of organic wastes in aqueous solution. A superior catalytic activity was obtained for PBC, which was much higher than that of the most popular Co3O4 nanocatalyst. More importantly, a detailed mechanism of PMS activation on the MIEC perovskite was proposed. Electron paramagnetic resonance (EPR) and radical competitive reactions suggested that both sulfate radicals (SO4•–) and hydroxyl radicals (OH) participated in and played important roles in the catalytic oxidation processes. Oxygen temperature-programmed desorption (O2-TPD) demonstrated that the PBC perovskite oxide is capable of facilitating an easier valence-state change of the B-site cation (cobalt ions) to mediate a redox process. Additionally, the oxygen vacancies could facilitate the bonding with PMS molecules and promote the reactivity of cobalt ions for PMS activation. Electrochemical impedance spectroscopy (EIS) was also performed to evidence charge transfer and surface reaction rates of the PBC catalyst that are much faster than those of Co3O4. Additionally, suppressed cobalt leaching was also achieved through tailoring the pH value of the reaction solution. This study provides insight into MIEC perovskites in catalytic reactions and applications.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.6b02303.

  • XRD patterns of PBC, H-Co3O4, and P-Co3O4; Rietveld refinement of XRD patterns for fresh PBC and after the O2-TPD test; SEM images of PBC and M-Co3O4; TEM images of H-Co3O4 and P-Co3O4; H2-TPR profile of PBC; TGA-DSC curves of Co3O4 and PBC; XPS spectra of Pr 3d on PBC before and after the phenol degradation test; relative concentrations of surface oxygen species; iodometric titration technique; methylene blue and phenol oxidation on various catalysts; first-order kinetic model of phenol oxidation on PBC, H-Co3O4, and P-Co3O4; the stability test of PBC for methylene blue degradation; the degradation of phenol without a catalyst or PMS (the initial pH value of the reaction solution was 9); and the calculations of turnover frequency (PDF)

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