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Tuning the Selectivity in the Aerobic Oxidation of Cumene Catalyzed by Nitrogen-Doped Carbon Nanotubes

Authors

  • Shixia Liao,

    1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)
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  • Yumei Chi,

    1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)
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  • Dr. Hao Yu,

    1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)
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  • Dr. Hongjuan Wang,

    1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)
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  • Prof. Dr. Feng Peng

    Corresponding author
    1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)
    • School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640 (China)

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Abstract

In this study it is demonstrated that carbon nanotubes (CNTs) with doped nitrogen atoms in graphitic domains (NCNTs) can act as a new class of metal-free catalysts exhibiting excellent activity in the aerobic oxidation of cumene. We proved that NCNTs can promote the decomposition of hydroperoxide cumene with exceptionally high activity, resulting in strongly increased cumene conversion and extraordinarily high selectivity to acetophenone and 2-benzyl-2-propanol. The incorporation of nitrogen altered the surface electron structure of the CNTs and tuned the reactivity and selectivity. DFT calculations revealed that the remarkable improvement of catalytic performance of NCNTs is caused by the strong interaction between hydroperoxide cumene and the NCNTs. NCNTs also exhibited desirable recyclability after four cycling tests. This study not only provides a novel method for the cumene oxidation to high-value-added products at moderate reaction temperatures and oxygen atmospheric pressure, but also gives new insights into the effect of surface nitrogen doping on carbon-catalyzed liquid-phase oxidation of aromatic hydrocarbons.

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