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Facile Synthesis of High-Performance Nitrogen-Doped Hierarchically Porous Carbon for Catalytic Oxidation

  • Zhe Yang
    Zhe Yang
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
    More by Zhe Yang
  • Xiaoguang Duan
    Xiaoguang Duan
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia
  • Jun Wang
    Jun Wang
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
    More by Jun Wang
  • Yang Li
    Yang Li
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
    More by Yang Li
  • Xiaobin Fan
    Xiaobin Fan
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
    More by Xiaobin Fan
  • Fengbao Zhang
    Fengbao Zhang
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
  • Guoliang Zhang
    Guoliang Zhang
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
  • , and 
  • Wenchao Peng*
    Wenchao Peng
    School of Chemical Engineering and Technology, Tianjin University, 135 Yaguan Road, Tianjin 300050, China
    *Email: [email protected]. Tel.: 86-22-85356119.
    More by Wenchao Peng
Cite this: ACS Sustainable Chem. Eng. 2020, 8, 10, 4236–4243
Publication Date (Web):February 26, 2020
https://doi.org/10.1021/acssuschemeng.9b07469
Copyright © 2020 American Chemical Society
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Abstract

Carbonaceous materials are emerging metal-free catalysts for advanced water purification without secondary pollution. In this study, nitrogen-doped and hierarchically porous carbons with ultrahigh specific surface areas (SSAs) (>4500 m2 g–1) are fabricated using sodium nitrate (NaNO3) as a template and polyacrylamide as nitrogen and carbon precursors. Highly hierarchical porous structures can be created with uniform-dispersed macropores (50∼200 nm), mesopores (2∼4 nm), and micropores (0.7∼1.2 nm). These materials are then employed as metal-free catalysts for catalytic oxidation of phenol with peroxymonosulfate (PMS). The system demonstrates an outstanding catalytic activity with a rate constant of 0.622 min–1, outperforming many metal-based (Fe2+, Co2+, and Ag+) homogeneous systems. The catalytic mechanism is investigated by electron paramagnetic resonance (EPR) and radical quenching tests. The nonradical pathway contributed to the majority of phenol oxidation and to the minor amounts of SO4•–, •OH, and O2•– are also detected. The ultrahigh catalytic activity of the carbocatalysts results from the large SSA, nitrogen modification, abundance of defective sites, and functional groups. This salt-templating method is facile and generates high quality samples without residual template. The approach has a great potential for the practical production of low-cost, high-performance, and functional carbon materials for wastewater treatment. This work also provides new insights into metal-free catalysis in PMS activation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.9b07469.

  • XRD patterns of PAM-0-700, PAM-0.1-700, PAM-0.3-700, and PAM-0.5-700; EDS spectra of PAM-0.3-700 and PAM-0.5-700; BPA and 2,4-DCP removals on PAM-0.5-700; stability tests of PAM-0.5-700; C 1s and N 1s high-resolution scans of PAM-0.5-700 before and after reaction; XRD patterns of PAM-0.5-700 before and after reaction; Raman spectra of PAM-0.5-700 before and after reaction; SEM images of PAM-0-700 and PAM-0.5-700; and catalytic activity comparison with reported catalysts (PDF)

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