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Dimethyl Carbonate Are Researched Form Carbon Dioxide And Methanol On Copper-based Catalyst

Posted on:2014-08-11Degree:MasterType:Thesis
Country:ChinaCandidate:L WangFull Text:PDF
GTID:2251330401456617Subject:Physical chemistry
Abstract/Summary:PDF Full Text Request
Dimethyl carbonate (DMC) is a new type of environment-friendly organicsynthesis intermediates, It can replace the highly toxic chemicals such as dimethylsulfate, methyl chloride as the methylating reagent, can also replace the phosgene usedas a carbonyl reagent. In addition, DMC added to gasoline can not only improve theoctane number of the fuel, but also can reduce air pollution. CO2is the main cause ofglobal warming gas, is one of a stock of a lot of potential carbon resources. CO2andCH3OH was synthesized carbonate of dimethyl (DMC) with green chemistry andresource re-use of double meaning. This system of gas-solid reaction of CO2andmethanol direct synthesis of DMC.This article describes the CuxOy/ZnO-Al2O3catalyst and CeO2modified carrierafter CuxOy/ZnO-Al2O3-CeO2of catalyst and H-type zeolite modifiedCu/ZnO-Al2O3-CeO2/zeolite catalysts. Three types of catalytic activity and activitycenter, and the H-modified zeolite catalyst structure and the amount of acid werestudied, the DMC reaction conditions for gas-solid CO2and methanol synthesis arediscussed. Start work as follows:1It flow co-precipitation method and impregnation method to preparedCuxOy/ZnO-Al2O3catalyst, CeO2modified its carrier, and then the modification ofHZSM-5catalyst. Through the catalytic activity of the copper-based catalyst HZSM-5modified catalytic performance best, methanol conversion rate of7.98%. And dispersityincrease the active ingredient, the active ingredient grains smaller than the surface areaof the catalyst increases, the pore diameter becomes smaller, and the active ingredient isuniformly dispersed in the surface of the molecular sieve.2H2-TPR and XPS characterization results can calculate the content of eachcomponent in the active center CuxOy/ZnO-Al2O3catalyst. The three catalysts elementalcopper content was significantly higher than other copper oxide content. With elementalcopper content increases, the reduction in the content of copper oxide and cuprous oxide,the methanol conversion gradually increases.3HMCM-22HMCM-56, the hydrogen zeolite HZSM-5three kinds of catalyst C/ Z-A-Ce were modified, and three catalytic activity were compared. Over XRD and TPDcharacterization methods modified three catalysts were characterized by the activecomponent is highly dispersed in the surface of the carrier, and the greater the amountof surface acid catalyst, the better the catalytic performance. Using C/Z-A-Ce/HZSM-5catalyst ScS the reaction conditions of the system to determine the optimal reactionconditions for the system as follows: reaction pressure as1.0MPa, the reactiontemperature is230℃, the catalyst inputs for1.0g, CO2and CH3OH molar ratio of3:1.
Keywords/Search Tags:Dimethyl carbonate, Methanol, CuxOy/ZnO-Al2O3-CeO2/HZSM-5, Copper-based catalyst
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