Preparation Of Ordered Mesoporous Carbon Embedded With Copper Nanoparticles Materials And Its Application In Electrocatalytic Synthesis Of Benzyl Methyl Carbonate

Organic carbonates are organic compounds with a wide range of application and can be synthesized by non-electrochemical methods and electrochemical methods.The electrochemical method for preparing organic carbonates has the advantages of mild reaction conditions,simple equipment,controllable reaction,"green"reaction and so on,so this method has attracted much attention.One of the synthetic route of organic carbonates is electrocatalytic reaction of alcohol with CO₂.It uses the greenhouse gas CO₂ as raw material which not only can reduce the concentration of CO₂ in the atmosphere,but also can convert CO₂ into more valuable chemicals.At present,there have been many articles reporting electrocatalytic reaction of alcohols?monoalcohols,diols and triols?and CO₂ to synthesize organic carbonates.A part of investigations suggest that the reaction requires using toxic and harmful bases or cocatalysts and taking long reaction time,so it has the disadvantage of polluting the environment and consuming time;a part of investigations suggest that in the case of ionic liquid as solvent and without base and any cocatalyst,the reaction has high yield and the ionic liquid can be recycled,but the recycling process is complex;in those reports the working electrodes used are normally plate electrodes that show poor electrocatalytic performance.Therefore,it is very important to find a green synthetic route,a simple synthesis process to prepare an electrode material with good electrocatalytic performance.In general,the electrocatalytic performance of the electrode is proportional to the number of active sites,and metal in the form of nanoparticles disperse to support with high specific surface area can increase the number of active sites.Ordered mesoporous carbon has high specific surface area and pore volume.As support,the metal nanoparticles can be highly dispersed;as adsorbent,it has large gas adsorption capacity and a higher gas adsorption capacity after the N doping;regular ordered pore structure facilitates the diffusion of reactants;good stability and conductivity make it apply to the aspect of electrochemistry.Ordered mesoporous carbon is mostly used in lithium ion batteries,fuel cells and capacitors,and has rarely been reported in organic electrocatalytic synthesis.In this thesis,combing with the structural advantages of ordered mesoporous carbon and the technical advantages of organic electrocatalytic synthesis,the ordered mesoporous carbon is used as support to load with copper nanoparticle and dope N atom to prepare Cu/OMC electrode materials with highly dispersed copper nanoparticles and Cu/NMC electrode materials with higher CO₂ adsorption performance.They were applied to electrocatalytic reaction of benzyl alcohol with CO₂to synthesize benzyl methyl carbonate,and then the electrolysis conditions were optimized to investigate the factors affecting the electrocatalytic performance of the electrode materials.The electrolysis process avoids the use of alkali and cocatalyst,and is easy to operate,that overcomes the disadvantages of contamination environment,cumbersome operation and poor catalytic performance of plate electrodes.The specific research contents are as follows:?1?The Cu/OMC electrode materials were prepared by a simple and convenient one-pot method,and its characterization and electrocatalytic application were carried out.The study shows that the content of copper and the amount of acetylacetone added have a great influence on the structure and morphology of the material?the size of copper nanoparticles,specific surface area and pore volume of materials?and electrocatalytic performance of the electrode material.Electrolytic conditions such as current density,substrate concentration,and electrolysis were also investigated.It is proved that the electrocatalytic performance of Cu/OMC electrode material is better than that of the normally plate copper electrode.?2?On the basis of the research of Cu/OMC electrode materials,in order to improve the CO₂ adsorption performance of the material,Cu/NMC materials were prepared by a one-pot method,and their characterization and electrocatalytic applications were carried out.In the preparation process,N-vinylformamide is added as a chelating agent and an N source,and N-doping of the material is also achieved while dispersing the copper nanoparticles.Characterization proves that the N doping amount affects the pore structure,specific surface area,and pore volume of the material.The larger the specific surface area and the pore volume,the more the N doping amount,the better the CO₂ adsorption performance of the material.The electrocatalytic effect proves that the Cu/NMC electrode material has better electrocatalytic performance than Cu/OMC,indicating that the CO₂ adsorption performance of the material affects the electrocatalytic performance of the electrode material.