Selective Degradation of Organic Pollutants Using an Efficient Metal-Free Catalyst Derived from Carbonized Polypyrrole via Peroxymonosulfate Activation

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School of Environmental Science and Engineering, School of Chemistry and Chemical Engineering, and §Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, China
Department of Civil and Environmental Engineering, Rice University, Houston, Texas 77005, United States
*Phone: 86-21-54747354; fax: 86-21-54740825; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2017, 51, 19, 11288–11296
Publication Date (Web):August 31, 2017
https://doi.org/10.1021/acs.est.7b03014
Copyright © 2017 American Chemical Society
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Abstract

Metal-free carbonaceous materials, including nitrogen-doped graphene and carbon nanotubes, are emerging as alternative catalysts for peroxymonosulfate (PMS) activation to avoid drawbacks of conventional transition metal-containing catalysts, such as the leaching of toxic metal ions. However, these novel carbocatalysts face relatively high cost and complex syntheses, and their activation mechanisms have not been well-understood. Herein, we developed a novel nitrogen-doped carbonaceous nanosphere catalyst by carbonization of polypyrrole, which was prepared through a scalable chemical oxidative polymerization. The defective degree of carbon substrate and amount of nitrogen dopants (i.e., graphitic nitrogen) were modulated by the calcination temperature. The product carbonized at 800 °C (CPPy-F-8) exhibited the best catalytic performance for PMS activation, with 97% phenol degradation efficiency in 120 min. The catalytic system was efficient over a wide pH range (2–9), and the reaction of phenol degradation had a relatively low activation energy (18.4 ± 2.7 kJ mol–1). The nitrogen-doped carbocatalyst activated PMS through a nonradical pathway. A two-step catalytic mechanism was extrapolated: the catalyst transfers electrons to PMS through active nitrogen species and becomes a metastable state of the catalyst (State I); next, organic substrates are oxidized and degraded by serving as electron donors to reduce State I. The catalytic process was selective toward degradation of various aromatic compounds with different substituents, probably depending on the oxidation state of State I and the ionization potential (IP) of the organics; that is, only those organics with an IP value lower than ca. 9.0 eV can be oxidized in the CPPy-F-8/PMS system.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b03014.

  • Additional details on synthesis procedure and characterization of materials, HPLC analytic conditions and ionization potentials, additional characterization results and catalytic experiments, EPR spectra, reusability of the catalysts, relationships between adsorption or ionization potential and degradation of various aromatic compounds, and HPLC patterns. (PDF)

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