• 文献标题:   Selective Etching of N-Doped Graphene Meshes as Metal-Free Catalyst with Tunable Kinetics, High Activity and the Origin of New Catalytic Behaviors
  • 文献类型:   Article
  • 作  者:   DAI YQ, ZHOU J, HUANG CQ, GU Q, ZENG Y, XU WL, MENG XY, FU WL, SUN YM
  • 作者关键词:   4nitrophenol, graphene oxide, hydrogenation reaction, ndopant, substitutional doping
  • 出版物名称:   PARTICLE PARTICLE SYSTEMS CHARACTERIZATION
  • ISSN:   0934-0866 EI 1521-4117
  • 通讯作者地址:   Southeast Univ
  • 被引频次:   5
  • DOI:   10.1002/ppsc.201700395
  • 出版年:   2018

▎ 摘  要

New N-doped reduced graphene oxide (N-RGO) meshes are facile fabricated by selective etching of 3-5 nm nanopores, with controllable doping of N dopants at an ultrahigh N/C ratio up to 15.6 at%, from pristine graphene oxide sheets in one-pot hydrothermal reaction. The N-RGO meshes are illustrated to be an efficient metal-free catalyst toward hydrogenation of 4-nitrophenol, with new catalytic behaviors emerging in following three aspects: (i) tunable kinetics following pseudofirst order from commonly observed pseudozero order; (ii) strikingly improved activity with 26-fold increased rate constant (1.0 s(-1) g(-1) L); (iii) no induction time required prior to reaction due to depressed back conversion, and dramatically decreased apparent activation energy (E-a) (17 kJ mol(-1)). The origin of these new catalytic properties can be assigned to the synergetic effects between graphitic N doping and structural defects arising from nanopores. Deeper understanding unveils that the concentration of graphitic N is inverse proportion to E-a, while the pyrrolic N has no impact on this reaction, and oxygenate groups hampers it. The porous nature allows the N-RGO meshes to conduct catalyze reactions in continuous flow fashion.