The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis

  • Wei Ren
    Wei Ren
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA5005, Australia
    More by Wei Ren
  • Gang Nie
    Gang Nie
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA5005, Australia
    More by Gang Nie
  • Peng Zhou
    Peng Zhou
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA5005, Australia
    College of Architecture & Environment, Sichuan University, Chengdu 610065, China
    More by Peng Zhou
  • Hui Zhang*
    Hui Zhang
    Department of Environmental Science and Engineering, Wuhan University, Wuhan 430079, China
    *(H.Z.) Email: [email protected]
    More by Hui Zhang
  • Xiaoguang Duan*
    Xiaoguang Duan
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA5005, Australia
    *(X.D.) Email: [email protected]
  • , and 
  • Shaobin Wang
    Shaobin Wang
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA5005, Australia
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2020, 54, 10, 6438–6447
Publication Date (Web):April 17, 2020
https://doi.org/10.1021/acs.est.0c01161
Copyright © 2020 American Chemical Society
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Abstract

Persulfates activation by carbon nanotubes (CNT) has been evidenced as nonradical systems for oxidation of organic pollutants. Peroxymonosulfate (PMS) and peroxydisulfate (PDS) possess discrepant atomic structures and redox potentials, while the nature of their distinct behaviors in carbocatalytic activation has not been investigated. Herein, we illustrated that the roles of nitrogen species in CNT-based persulfate systems are intrinsically different. In PMS activation mediated by nitrogen-doped CNT (N-CNT), surface chemical modification (N-doping) can profoundly promote the adsorption quantity of PMS, consequently elevate potential of derived nonradical N-CNT–PMS* complexes, and boost organic oxidation efficiency via an electron-transfer regime. In contrast, PDS adsorption was not enhanced upon incorporating N into CNT due to the limited equilibrium adsorption quantity of PDS, leading to a relatively lower oxidative potential of PDS/N-CNT system and a mediocre degradation rate. However, with equivalent persulfate adsorption on N-CNT at a low quantity, PDS/N-CNT exhibited a stronger oxidizing capacity than PMS/N-CNT because of the intrinsic higher redox potential of PDS than PMS. The oxidation rates of the two systems were in great linearity with the potentials of carbon–persulfate* complexes, suggesting N-CNT activation of PMS and PDS shared the similar electron-transfer oxidation mechanism. Therefore, this study provides new insights into the intrinsic roles of heteroatom doping in nanocarbons for persulfates activation and unveils the principles for a rational design of reaction-oriented carbocatalysts for persulfate-based advanced oxidation processes.

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  • The approaches of electrochemical analysis. The method of phenol degradation. The degradation curves of phenol, persulfate adsorption curves, and potential of complexes in the persulfate/CNT and persulfate/N-CNT systems. Raman, XPS, and EIS spectra of N-CNT (PDF)

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