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1、ChemicalEngineeringScience59(2004)5509–5517www.elsevier.com/locate/cesDirectgas-phaseepoxidationofpropenewithnitrousoxideovermodifiedsilicasupportedFeOxcatalystsE.Ananieva,A.Reitzmann∗InstituteofChemicalProcessEngineering,UniversityofKarlsruhe(TH),Kaiserstr.12,76185K
2、arlsruhe,GermanyReceived29February2004AbstractVapourphaseepoxidationofpropenewithnitrousoxideoveralkalinecontainingsilicasupportedironoxidecatalystswasexperimentallyinvestigated.Areactionnetworkisdeducedfromthetrendsofproductselectivitiesasfunctionofpropeneconversio
3、nusingdifferentcatalysts.Importantsidereactionsareparallelpropanalformationandconsecutiveisomerisationsofpropyleneoxide(PO)topropanal,acetoneandallylalcohol.Ratesofthesereactionswereaffectedbycatalystcomposition,whichinfluencedacid-baseproperties,numberofsilanolgroup
4、sandsurfacearea.APOselectivityof∼75%andPOspace–timeyieldsof0.02–0.03g−1−1POgcathwereobtainedwithacatalystcontainingironoxo-speciesandcaesiumions/-oxides.TheseresultscanonlybeobtainedatahighsurplusofN2Oversuspropeneconcentrationinthereactorfeed.Likelyreasonsforthatis
5、aninhibitionofpropyleneoxide’sformationratebypropeneandpropyleneoxideitself.2004ElsevierLtd.Allrightsreserved.Keywords:Catalysis;Nitrousoxide;Propyleneoxide;Partialoxidation;Ironoxide;Reactionnetwork1.Introduction(e.g.ethylbenzene,isobutane).Afterseparateoxidationt
6、operoxides,thesecompoundsareusedasoxygendonorsforWithaworldwideproductioncapacityofmorethan5×thepropeneepoxidation(Arpentinieretal.,2001).Although106tonsperyearandpositivemarketforecast,propylenetheseco-reactantsaresubsequentlyconvertedtomarketableoxide(PO)represent
7、sanimportantchemicalintermediateproducts,processeconomyofPOsynthesisextremelyde-withgrowingattention(Haasetal.,2001).However,twopendsonmarketpricesofcoupledproducts.Awareofthisunsatisfyingroutesinliquidphase,theso-calledchlorhy-problem,SUMITOMOusescumeneasco-reactan
8、twhichisdrinprocessandtheperoxidationprocess,arestillprevail-recoveredandrecycledafterhydrogenationofthecoupledinginPOsproductiontechnolog
