Green Energy & Environment (Oct 2020)

Active sites and reaction mechanism for N-doped carbocatalysis of phenol removal

  • Mingjie Zhang,
  • Chen Han,
  • Wenyao Chen,
  • Wei Luo,
  • Yueqiang Cao,
  • Gang Qian,
  • Xinggui Zhou,
  • Xiaoguang Duan,
  • Shaobin Wang,
  • Xuezhi Duan

Journal volume & issue
Vol. 5, no. 4
pp. 444 – 452

Abstract

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Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance. Herein, the underlying nature of N promotional effects on peroxymonosulfate (PMS) activation for phenol removal is understood by combining kinetics analysis with multiple techniques. A strategy using mixed acid oxidation of carbon nanotube (CNT) followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp2-hybridized carbon and defective degree, endowing with a chance to discriminate the dominant N-containing active sites. The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites. The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism. The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.

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