若干介孔分子篩的合成、表征及其催化反應(yīng).pdf

1、復(fù)旦大學(xué)碩士學(xué)位論文若干介孔分子篩的合成、表征及其催化反應(yīng)姓名：任瑜申請學(xué)位級別：碩士專業(yè)：物理化學(xué)指導(dǎo)教師：賀鶴勇20030516若千介孔分子篩的合成、表征和催化反應(yīng)AbstractZeolitehasbeenwidelyusedincatalysisbecauseofitsspecialporestructureandlargesurfacearea.Howeverthesmallporesizerestrictsitusedinc

2、atalyticreactionsinvolvinglargemolecules.AlthoughthediscoveryofM41Smesoporousmolecularsievesopenedanewwayincatalysistherelativelylowacidityandhydrothermalstabilityofmesoporousmolecularsievesisnotdesirableincatalyticappli

3、cation.InthisdissertationweusedtheethylamineandCTABasthecotemplatetosynthesizeMCM41mpwhichcontainsmicroporousandmesoporousstructures.Theintroductionofmicroporeinmesoporousmaterialsincreasesthehydrothermalstability.Thedis

4、coveryoftheTicontainingmolecularsieveTSIhasledtoconsiderableinterestinliquidphaseselectiveoxidationcatalysisusingaqueoushydrogenperoxideasanenvironmentallyfriendlyoxidant.HowevertheporesizeofclassicalTicontainingmicropor

5、ousmolecularsievesrestrictsthetypeofmoleculeswhichcanaccessthezeoliteintracrystallinevoidspacewherecatalysisoccurs.Ticontainingmesoporousmolecularsievemayaccommodatelargemolecules.Butitsuferseitherlowreactionperformanceo

6、rcomplicatedsynthesisprocedures.InthisdissertationwedevelopedaneasywaytodirectlyintroducehighlyactivetetrahedralTi`centersintomesoporoussilicathrough“onepotconversion“usingshortchaincarboxylicacidsasthetemplates.Thiskind

7、oftitanosilicatehaswormlikethreedimensionalporestructure.Ithasaconversionof80.7%andselectivityof91.5%intheepoxidationreactionofcyclohexeneWealsousethissolgelmethodtosuccessfullysynthesizemesoporoussilicacontainingotherme

8、talactivespeciessuchasFeCuMoZrNiMn.Thesecatalystsshowhighperformanceofthereactionofphenolhydroxylation.AmongwhichFecontainingmesoporoussilicacatalysthasaconversionof27.2%andselectivityof100.0%todiphenolandCucontainingone