Preparation Of Functionalized Carbon Materials For Liquid Phase Oxidation And Reduction

Precious metals are expensive and their storage is limited.So,developing non-precious metal and non-metallic catalysts to replace precious metal catalysts is of great importance to modern industrial development.Heteroatom-doped functionalized carbon materials have unique properties and are widely applied in the fields of electrochemistry,photocatalysis,and traditional catalysis.However,the processes of synthesis and functionalization of carbon materials often require relatively cumbersome steps.Based on this situation,we developed a simple synthesis method to prepare heteroatom-doped carbon material catalysts,and studied the catalytic active sites and catalytic mechanism.The main findings are as follows:(1)B/N co-doped carbon material with high surface area(1100-1400 m~2/g)and micro,mesoporous structure was synthesized with chitin as precursor.The carbon material exhibited excellent catalytic activity in the catalytic oxidation of ethylbenzene.The experimental results and theoretical calculations showed that the boron nitride microdomain in the catalyst is catalytic active center.(2)B/N co-doped carbon material(BNC)was synthesized using boric acid and ammonia triacetic acid(NTA)as precursors,and employed as a metal-free catalyst for the hydrogenation of nitroaromatics.It exhibited outstanding catalytic activity under mild reaction conditions(yield:52.1-100%).Experimental results,characterization analyses and DFT theoretical calculations showed that the synergistic effect between B and N heteroatoms in the carbon material is a key factor for its high catalytic activity.(3)Magnetic nitrogen-containing carbon material was synthesized by hydrothermal method using N-Acetyl-D-glucosamine(NAG)and ferric nitrate as raw materials,and explored its catalytic performance in the epoxidation of stilbene.Studies showed that nitrogen species located in graphite carbon skeleton is a key factor to promote the catalytic oxidation of C-H,the iron species in the material is indispensable for the catalytic performance of catalyst.