1、天津大學(xué)博士學(xué)位論文氧化鈰催化CO2和甲醇直接反應(yīng)合成碳酸二甲酯姓名：王瑋申請(qǐng)學(xué)位級(jí)別：博士專業(yè)：化學(xué)工程與技術(shù)；化學(xué)工藝指導(dǎo)教師：馬新賓201105ABSTRACTDimethylcarbonate(DMC)h嬲beenwidelyusedas繃enVironmentallybenignintc冊(cè)ediateinchemicalinduSt拶forthercplacementofphosgeneforpolycarbbnateprod

2、uctionandotherprocessesoverthepastyears，DMChasbeenconsidercdasaideaIcandidatefor他placingmethylfP，，butylether(MTBE)嬲theadditivet0gasolineandtheutiIizationofDMCexhibitsexcellentprospectsCarbondioxide，whichcon仃ibutest0thein

3、crcaseinglobaItcmpemturesandtheclimatechangeduet0thegreenhouseeffe吒hasattractedconsiderableattentionforthechemicalutilizationT_lleprocessfordirectsynthesisofDMC行omC02andmeth鋤olnotonlyproduceseconomicchemicalswithhi曲Value

4、，butals0benefitsfortheenvironmentbyusingC02鷸a他cycledcarbonresourceDirectsynthesisofDMC仔omC02卸dmethanoloVerceriumoxidewasstudiedsystematicallyinthisdissertationC0mbiningtheNH3／C02一TPD陀sultswithcataI”icpe晌舯anceofCe02calcin

5、edatdifferenttempe仡tures，itissuggeStedthatthemoderateacidsiteswithdesorptionpeakofNH3一TPDat340℃exhibit鋤excellentcataI”icfomationofDMC鋤da他themain∞tiVe∞idsitesThemoderateacidsiteswithdesorptionpeakat260℃areunfavorableforth

6、esynthesisofDMCandthestrongacidsiteshavenodi他Ctimpactsonthecatal”icactiVityComparedt0thebasesites，the∞idsitesonthesurl’aceofCe02arethemainfacto體whichafI宅ctthecatal”icperfonnanceThec巧stalofCe02hasthes仃uctureofcubicfluorit

7、ewiththeprima噦characteriSticsurf≥Icesof(111)，(110)and(100)Duetothedif詫rencesinthepackingofatomsinbulk蛐mctureandcenainlyatsurface，theinteractionforcesbetweenthesurfacesandthe他actantswouIdbediffercntBycontrollingtheconcent

8、rationofalkalisolutionandthercactiontemperaturc，Ce02withdia’erentmorphoIogiesw髂synthesizedthroughthehydrothe咖almethodCombiningwithHRTEM抽dSEAD，thesu嗍cesofCe02withdi舵rentmorphologieswereconfimedConnectedwiththecatal”icperf

9、0咖ance，itissuggeStedthatnanorodsexhibitthehi曲est他actiVityforthesynthesisofDMCand(1l0)isthemainactivesurfj蛇eNanocubesshowthelowest∞tiVityforthe他actionindicatingthat(100)surfaceshavelittleactivityforthesynthesisofDMCTheact