甲烷和二氧化碳在分子篩負載銠催化劑上的活化和反應研究.pdf

1、Y“／70638飯旦大學碩士學位論文學校代碼學號甲烷和二氧化碳在分子篩負載銠催化劑上的活化和反應研究院系(所)：化學系專業(yè)：姓名：指導教師：完成日期：物理化學錢林平賀鶴勇教授2005年5月22日1024602202203復旦大學碩士掌位論文AbstractItisachallengingprojectintheC1chemistryfortheconversionofmethaneandcarbondioxideintovaluable

2、productsMethaneandcarbondioxidearebothgreenhousegasandverydifficulttobeactivatediochemicalreactionsConversionofmethaneandcarbondioxideintosynthesisgasisaneffectivewayofthefunctionalizationofbothgasesHoweverthereactionreq

3、uireshightemperatureManyeffectshavebeenpaidinthestudyofhighlyeffectivecatalystsRecentyears，cortvarsionofmethaneandcarbondioxideundermildconditionsintooxygenatedproductsgivesanewwayfortheutilizationofbothgasesTheresearchi

4、nthisthesishasbeenconcentratedonthestudyofactivationofmethaneandcarbondioxideundermildconditionsbyinsitusolidstateNMRandIRspectroscopiesandthestudyofthedryreformingreactionofmethaneandcarbondioxideThemajorresultsarethefe

5、llows(1)Carbonexchangebetweenmethaneandcarbondioxidewasfoundundermildconditions(300。C)over2％RNHBEAthroughtheinvestigationofthereactionof”CH4andC02ThesimilarphenomenonwasalsofoundinthesystemofCH4and”C02Theresultsprovethat

6、thecarbonexchangereactionisreversibleTheequilibriumconstantequalstoca1如situFTIRwasfurtherusedtostudythecarbonexchangereactionandallintermediate，HnCO，wasfoundAreactionmechanismwasproposed(2)Thedryreformingofmethaneandcarb

7、ondioxideintosynthesisgaswasstudiedathi∞temperature(850。C)overHBEAsupportedRhcatalystTheyieldofCOreaches82％over2％Rh小BEAWithincreasingoftherhodiumcontent，theyieldofcarbonmonoxideincreasesAlso，theRh／HBEAcatalystexhibitshig

8、hcatalyticandstructuralstabilities(3)TheeffectofsupportwasinvestigatedinthedryreformingofmethaneandcarbondioxideintosynthesisgasAtthesamereactionconditiontheyieldsofcarbonmonoxideoverbothRNHBEAandRh／H—ZSM5weresimilar(ca8

9、0％)andthatoverRh／SBA15wasabove92％AlthoughtheaciditystrengthofSBA15ismuchweakerthanthoseforHBEAandH—ZSM5thehighyieldofcarbonmonoxideoverSBA15supportedcatalystindicatesthattheactivityofcatalystonreformingreactionisnotdirec