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2D N-Doped Porous Carbon Derived from Polydopamine-Coated Graphitic Carbon Nitride for Efficient Nonradical Activation of Peroxymonosulfate

  • Jie Miao
    Jie Miao
    School of Environmental Science and Engineering, Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, P. R. China
    More by Jie Miao
  • Wei Geng
    Wei Geng
    School of Environmental Science and Engineering, Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, P. R. China
    More by Wei Geng
  • Pedro J. J. Alvarez
    Pedro J. J. Alvarez
    Department of Civil and Environmental Engineering, Rice University, Houston, Texas 77005, United States
  • , and 
  • Mingce Long*
    Mingce Long
    School of Environmental Science and Engineering, Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, P. R. China
    *Tel: 86-21-5474-7354; fax: 86-21-5474-0825; e-mail: [email protected]
    More by Mingce Long
Cite this: Environ. Sci. Technol. 2020, 54, 13, 8473–8481
Publication Date (Web):June 8, 2020
https://doi.org/10.1021/acs.est.0c03207
Copyright © 2020 American Chemical Society
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Abstract

Nitrogen-doped carbon materials attract broad interest as catalysts for peroxymonosulfate (PMS) activation toward an efficient, nonradical advanced oxidation process. However, synthesis of N-rich carbocatalysts is challenging because of the thermal instability of desirable nitrogenous species (pyrrolic, pyridinic, and graphitic N). Furthermore, the relative importance of different nitrogenous configurations (and associated activation mechanisms) are unclear. Herein, we report a “coating-pyrolysis” method to synthesize porous 2D N-rich nanocarbon materials (PCN-x) derived from dopamine and g-C3N4 in different weight proportions. PCN-0.5 calcined at 800 °C had the highest surface area (759 m2/g) and unprecedentedly high N content (18.5 at%), and displayed the highest efficiency for 4-chlorophenol (4-CP) degradation via PMS activation. A positive correlation was observed between 4-CP oxidation rates and the total pyridinic and pyrrolic N content. These N dopants serve as Lewis basic sites to facilitate 4-CP adsorption on the PCN surface and subsequent electron-transfer from 4-CP to PMS, mediated by surface-bound complexes (PMS–PCN-0.5). The main degradation products were chlorinated oligomers (mostly dimeric biphenolic compounds), which adsorbed to and deteriorated the carbocatalyst. Overall, this study offers new insights for rational design of nitrogen-enriched carbocatalysts, and advances mechanistic understanding of the critical role of N species during nonradical PMS activation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c03207.

  • Texts S1, S3, and Figures S15–S17, characterization of catalysts and methods for intermediates detection during 4-CP oxidation; Text S2, activation evaluation; Table S1, HPLC conditions for different organic compounds; Tables S2–S6, Figures S1–S6, additional characterizations of catalysts; Figures S7 and S9–S14, additional catalytic tests; Figure S8, relationship between oxidation rates of 4-CP and contents of different N species or defects in as-prepared catalysts; Figures S18 and S19, recyclability tests and practical application of the catalysts (PDF)

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