▎ 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.