N-benzylidene aniline is an important fine intermediates.It is of great significance to research and develop new highly efficient catalysts to realize efficient catalytic synthesis of N-benzylidene aniline under mild conditions.In this thesis,nitrogen-doped carbon-supported copper nanocatalyst and nitrogen-doped carbon-supported cobalt nanocatalyst were prepared and used as catalysts for catalytic synthesis of N-benzylaniline without external hydrogenation source.The content of this thesis is shown below:(1)A series of nitrogen-doped carbon-supported copper nanocatalyst(Cu-N-C)was prepared and obtained through the procedure of amide polymerization and high annealing.The characterization of XRD,XPS,and TEM were employed to explore the structure and morphology of the catalyst Cu-N-C.The synthesis of N-benzylidene aniline from nitrobenzene and benzyl alcohol under nitrogen atmosphere was also studied.The results showed that with the optimum condition of 0.6 MPa N2,temperature of 160°C,reaction time of 24 h,and toluene solvent,the catalyst Cu0.1-N-C could catalyze the synthesis of N-benzylidene aniline with a yield of 84%.However,the recycle tests indicated that the loss of Cu nanoparticlesa out from the catalyst Cu0.1-N-C was inevitable,resulting in the decrease of its catalytic activity.(2)In order to improve the stability of the catalyst,a series of nitrogen-doped carbon-supported cobalt nanocatalyst was designed and obtained through the procedure of pre-polymerization and subsequent high annealing.The synthesis of N-benzylidene aniline from nitrobenzene and benzyl alcohol under nitrogen atmosphere was then studied.Under the optimum condition of 0.6 MPa N2,temperature of 140°C,reaction time of 12 h,and octane solvent,the Co-N-C/800catalyst could catalyze the synthesis of N-benzylidene aniline with a yield of 98%and remain good catalytic performance after five recycle runs.The control experiments result further indicated that the Co-N-C/800 catalyst had a large specific surface area and rich mesoporous structure.The support nitrogen-doped carbon material can disperse cobalt nanoparticles very well,which can effectively promote the interaction between reactants and cobalt metal active sites,and finally the excellent catalytic activity of Co-N-C/800 catalyst was achieved. |