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Potential Difference Driving Electron Transfer via Defective Carbon Nanotubes toward Selective Oxidation of Organic Micropollutants

  • Penghui Shao
    Penghui Shao
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Penghui Shao
  • Shuiping Yu
    Shuiping Yu
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Shuiping Yu
  • Xiaoguang Duan
    Xiaoguang Duan
    School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
  • Liming Yang
    Liming Yang
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Liming Yang
  • Hui Shi
    Hui Shi
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Hui Shi
  • Lin Ding
    Lin Ding
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Lin Ding
  • Jiayu Tian
    Jiayu Tian
    School of Civil Engineering and Transportation, Hebei University of Technology, Tianjin 300401, P. R. China
    More by Jiayu Tian
  • Lixia Yang
    Lixia Yang
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    More by Lixia Yang
  • Xubiao Luo*
    Xubiao Luo
    Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang 330063, P. R. China
    National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, P. R. China
    *Email: [email protected]
    More by Xubiao Luo
  • , and 
  • Shaobin Wang
    Shaobin Wang
    School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2020, 54, 13, 8464–8472
Publication Date (Web):June 10, 2020
https://doi.org/10.1021/acs.est.0c02645
Copyright © 2020 American Chemical Society
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Abstract

Nanocarbon-based persulfate oxidation emerges as a promising technology for the elimination of organic micropollutants (OMPs). However, the nature of the active site and its working mechanism remain elusive, impeding developments of high-performance oxidative technology for water treatment practice. Here, we report that defect-rich carbon nanotubes (CNTs) exhibit a superior activity in the activation of peroxymonosulfate (PMS) for OMP oxidation. Quantitative structure–activity relationship studies combined with theoretical calculations unveil that the double-vacancy defect on CNTs may be the intrinsic active site, which works as a conductive bridge to facilitate the potential difference-dominated electron transfer from the highest occupied molecular orbital of OMPs to the lowest unoccupied molecular orbital of PMS. Based on this unique mechanism, the established [email protected] oxidative system achieves outstanding selectivity and realizes the target-oriented elimination of specific OMPs in a complicated aquatic environment. This work sheds new light on the mechanism of carbocatalysis for selective oxidation and develops an innovative technology toward remediation of practical wastewater.

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