葡萄糖氧化酶活性中心与碳纳米电极相互作用的理论分析-theoretical analysis of interaction between glucose oxidase active center and carbon nano - electrode.docxVIP

ABSTRACTBiofuelcellsarethepowergenerationdevicesofusingenzymesormicroorganismsgroupasacatalysttoconvertchemicalenergyoffuelintoelectricity.Enzymebiofuelcellsareattractingwideattentioninrecentyears,ofwhichusingglucoseoxidaseasanodecatalystandglucoseasfuel.Therefore,thetheorystudyoftheinteractionbetweenglucoseoxidaseactivitycenter(flavin)andcarbonnanomaterialelectrodesisveryimportanttothedevelopmentofbiofuelcell.Thisworkincludesthreeparts：Thefirstpartisthetheorystudyoftheinteractionbetweenglucoseoxidaseactivitycenter(flavin)andthesurfaceofcarbonnanotubes(sCNT).Byusingdensityfunctionaltheory,thereductionstate,thehalfreductionstate,andtheoxidationstateofflavininteractedwithsCNTindifferentcouplingmodes,andthesystemisoptimizedinthetheorylevelofM062X/6-31+g(d).Weanalyzedthebindingenergy,electronclouddistribution,bandgap,densityofstateandotherpropertiesconcretely.StudieshaveshownthatthecombinationofflavinandsCNTisphysicaladsorption,vanderWaalsforceplaysthemainrole,andtheelectronclouddistributionisdifferentwhensCNTinteractwiththedifferentstatesofflavin.TheadsorptionofthereductionstateofflavinismostconducivetotheelectrontransferbetweenflavinandsCNT,secondisthehalfreductionstate,thelastistheoxidationstate.TheadsorptionofflavincanmaketheelectricalconductivityofsCNTenhanced.Theparallelcouplingmodeisbetterthanverticalcouplingmodebasedonbindingenergyandbandgapproperties.Thesecondpartisthein-depthstudyonthebasisofthefirstpart.Itisthetheorystudyoftheinteractionbetweenglucoseoxidaseactivitycenter(flavin)andcarbonnanotubes(CNT).TheproblemoftheinteractionbetweenCNTandflavinindifferentconformationswereanalyzedusingONIOMlayeredcalculationmethodofwhichthehigh-levelwiththeM062X/6-31+g(d)theoreticallevelandthelow-levelwiththeM062X/sto-3gtheoreticallevel.Wealsocalculatedthepropertiesofthebindingenergy,electronclouddistribution,bandgaps,densityofstate,andcomparedthemwiththefirstpart.Resultsshowthatitissametothefirstpart,theinteractionbetweenflavinandCNTisphysicaladsorptionwhetheritistheparall