Preparation And Application Of Porous Nitrogen-Doped Carbon-Based Catalyst

Heterogeneous catalysts are favored by chemists for their easy separation and recyclability in the reaction system,and porous heteroatom-doped carbon-based materials have been widely studied in heterogeneous catalytic reactions.This paper is divided into two parts to prepare transition metal-supported and non-metal-supported porous nitrogen-doped carbon materials and investigate the catalytic performance of synthesis imines.The main contents are as follows:1?The efficient and stable catalyst applied to the transformation of amines into the corresponding imines and hydrogenation of nitroarenes under mild reaction conditions is reported in the paper.The catalytic performance of porous N-doped carbon with FeCu?FeCu@NPC?catalyst are tested by aromatic alcohol and amine with solvent-free and hydrogenation of nitroarenes via N₂H₄·H₂O.The results proved that the yield of these two reactions are all over 99.9%under optimum condition.Moreover,the synergistic effect of the catalyst for synthetic imine reaction was investigated through the kinetic study.The catalyst can be easily separated from reaction system by an external magnetism,and can be recycled and reutilized for at least 4 runs without distinct activity reduction.The study of the catalyst indicated that it was suitable for the reactions in industry.In addition,in this work,we explored the active site of the catalyst and found that graphitic nitrogen in the material is one of the active components.2?We have successfully prepared carbon microsphere precursors using cheap melamine and 3-aminophenol as raw materials,and calcined them at a specific temperature to obtain mesoporous azacarbon materials?NC?for autooxidative coupling of primary amines.The obtained results showed that most of the yields of imines exceeded 90%,and the cycling performance of the catalyst could be at least seven runs without any decay in the reaction activity,which could be comparable to those of metal catalysts.Subsequently,a kinetic study has demonstrated that the apparent activation energy for the direct synthesis of imines from amines is 67.39 kJ mol^-1.And through the characterization and experimental data of the catalyst,the active site of graphite-N catalyst was further explained.