• 文献标题:   Metal-free catalytic ozonation on surface-engineered graphene: Microwave reduction and heteroatom doping
  • 文献类型:   Article
  • 作  者:   WANG YX, CAO HB, CHEN CM, XIE YB, SUN HQ, DUAN XG, WANG SB
  • 作者关键词:   metalfree oxidation, ndoping, microwave, defect, catalytic ozonation
  • 出版物名称:   CHEMICAL ENGINEERING JOURNAL
  • ISSN:   1385-8947 EI 1873-3212
  • 通讯作者地址:   Chinese Acad Sci
  • 被引频次:   23
  • DOI:   10.1016/j.cej.2018.08.134
  • 出版年:   2019

▎ 摘  要

N-doped graphene has demonstrated exceptional activities in versatile metal-free catalytic processes. In this study, reduced graphene oxide (rGO) and N-doped rGO were synthesized by a facile approach via microwave reduction with a low energy input and short reaction time. The activities of the derived carbocatalysts were evaluated by catalytic ozonation of 4-nitrophenol (4-NP). Compared with thermally annealed rGOs in argon atmosphere, microwave treated rGO demonstrated a better performance in catalytic oxidation, and N-doping would further improve the catalytic activity. It is discovered that microwave irradiation not only gave rise to more edging sites and dangling bonds in rGO, making higher catalytic potentials for ozone decomposition than that from thermal annealing, but also resulted in a higher concentration of N dopants. XPS studies revealed that more graphitic N species were incorporated into the carbon basal plane during the microwave reduction processes. The reactive oxygen species (ROS) in 4-NP oxidation were evaluated and identified by liquid-phase electron spin resonance (ESR) and radical scavenging tests, which indicated the generation of O-2(center dot-), center dot OH and O-1(2) for 4-NP degradation. This study provides a facile protocol for fabricating advanced nanocarbon materials for green oxidation and enables new insights in catalytic ozonation with state-of-the-art carbocatalysis.