4.7 Article

Unprecedented Nonphotomediated Hole (h+) Oxidation System Constructed from Defective Carbon Nanotubes and Superoxides

期刊

ACS CENTRAL SCIENCE
卷 7, 期 2, 页码 355-364

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.0c01600

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资金

  1. National Natural Science Foundation [21806192, 21527813, 21737006]
  2. Natural Science Foundation of Guangdong Province [2018A030313441]
  3. Fundamental Research Funds for the Central Universities [19lgpy135]
  4. Jiangsu Key Laboratory of Vehicle Emissions Control [OVEC053]

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This study reports an unprecedented non-photomediated hole oxidation system constructed from carbon nanotubes and superoxides, which exhibits high catalytic activity for the degradation of organic pollutants. This finding opens up new research directions in the fields of environmental remediation, chemical synthesis, and biology.
Holes (h(+)) on heterogeneous photocatalysts could act as important oxidative species or precursors for reactive oxygen species (ROS). However, due to the ultrafast recombination of photoinduced electrons and holes, a majority of carriers are consumed prior to surface reactions. Herein, we report an unprecedented non-photomediated hole oxidation system constructed from carbon nanotubes (CNTs) and superoxides. This system exhibited high catalytic activity for the degradation of organic pollutants, which outperforms the classical oxidation processes in the remediation of actual wastewater and is comparable to that of the best single cobalt atom catalyst. Theoretical and experimental results reveal that the intrinsic defects with unpaired spins on CNTs served as adsorptive sites to activate superoxides. This is the first report on exploring the oxidation properties of nonphotomediated hole carriers on heterogeneous catalysts, which will be of broad interest for researchers in environmental remediation, chemical synthesis, and biological fields.

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