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Efficient Catalytic Ozonation over Reduced Graphene Oxide for p-Hydroxylbenzoic Acid (PHBA) Destruction: Active Site and Mechanism

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Division of Environment Technology and Engineering, Beijing Engineering Research Center of Process Pollution Control, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
§ University of Chinese Academy of Sciences, Beijing 100049, China
*Email: [email protected] (H.C).
*Email: [email protected] (S.W).
Cite this: ACS Appl. Mater. Interfaces 2016, 8, 15, 9710–9720
Publication Date (Web):March 23, 2016
https://doi.org/10.1021/acsami.6b01175
Copyright © 2016 American Chemical Society
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Abstract

Nanocarbons have been demonstrated as promising environmentally benign catalysts for advanced oxidation processes (AOPs) upgrading metal-based materials. In this study, reduced graphene oxide (rGO) with a low level of structural defects was synthesized via a scalable method for catalytic ozonation of p-hydroxylbenzoic acid (PHBA). Metal-free rGO materials were found to exhibit a superior activity in activating ozone for catalytic oxidation of organic phenolics. The electron-rich carbonyl groups were identified as the active sites for the catalytic reaction. Electron spin resonance (ESR) and radical competition tests revealed that superoxide radical (O2) and singlet oxygen (1O2) were the reactive oxygen species (ROS) for PHBA degradation. The intermediates and the degradation pathways were illustrated from mass spectroscopy. It was interesting to observe that addition of NaCl could enhance both ozonation and catalytic ozonation efficiencies and make ·O2 as the dominant ROS. Stability of the catalysts was also evaluated by the successive tests. Loss of specific surface area and changes in the surface chemistry were suggested to be responsible for catalyst deactivation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.6b01175.

  • SEM images, N2 adsorption, XPS spectra and surface acidic/basic sites of the samples, variation of ozone concentration during the experiments, kinetic studies in effects of some reaction conditions and MS spectra of reaction intermediates (PDF).

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