合成甘油碳酸酯体系的液液相平衡与cao基催化剂分析-liquid - liquid equilibrium and cao - based catalyst analysis of glycerol carbonate synthesis system.docxVIP

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合成甘油碳酸酯体系的液液相平衡与cao基催化剂分析-liquid - liquid equilibrium and cao - based catalyst analysis of glycerol carbonate synthesis system.docx

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合成甘油碳酸酯体系的液液相平衡与cao基催化剂分析-liquid - liquid equilibrium and cao - based catalyst analysis of glycerol carbonate synthesis system

AbstractGlycerolcarbonate,agreenchemical,isakindoforganicchemicalrawmaterialswidelyused.Itismainlyusedasreactionintermediatesandsolvents,orreactswithisocyanate,acrylicesterproductsandproductpolymertouseincoating,adhesiveandlubricantandsoon.thisdissertationisbasedonthetransesterificationofDMCandmethanoltoproduceGlycerolcarbonate,andmainlyfocusedontheresearchforthermodynamicsandcatalystsaboatthissystemtolaythefoundationforthedevelopmentofsubsequentsynthesisprocessofglycerolcarbonate.Liquid–liquidequilibria(LLE)dataoftheternarysystemdimethylcarbonate+methanol+glycerolweremeasuredfrom303.15Kto333.15K.TheequilibriumdataarecorrelatedwiththeNRTLandUNIQUACmodel.Thereliabilityofthismodelistestedbycomparisonwiththeexperimentalresults.Ontheotherhand,LLEandvapor–liquidequilibria(VLE)ofthebinarysystemdimethylcarbonate+glycerolwerealsomeasuredunderisopiesticpressure(101.3kPa)andpredictedusingtheNRTLmodel,withtheadjustedparametersobtainedfromtheLLEdataoftheternarysystemdimethylcarbonate+methanol+glycerol.ThepredictedVLEandLLEforthebinarysystemagreedwellwiththeexperimentaldata.TheextrudedCaO-basedcatalystswerepreparedandusedforthesynthesisofglycerolcarbonatefromglycerolanddimethylcarbonate.Theeffectsofbinders(diatomite,kaolin,andactivatedalumina),pore-formingagents(polyacrylamide,activatedcarbon,andpolyethyleneglycol),andcalcinationtemperatures(700oC,800oC,and900oC)onthecatalyticactivityandstabilityofthecatalystwereinvestigated.XRD,FT-IR,BET,andSEMwereusedforthecharacterizationofthepreparedcatalyst.ItwasfoundthattheinitialactivityofthefreshextrudedCaO-basedcatalystislowerthantheCaOpowdercatalystbecauseoftheresistanceoftheinternaldiffusion;however,thestabilityoftheformerwasfarbetterthanthelatter.Usingactivatedaluminaasthebinderandpolyacrylamideasthepore-formingagent,underthe3:1ofCaO/bindermassratio,800oCofcalcinationtemperature,and80oCofreactiontemperature,theglycerolconversionandglycerolcarbonateyieldcouldreach95.39%and90.57%forthefreshcatalystand65.47%and62.53%fortherecoveredcatal