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1、PublishedonWeb02/11/2010EvolutionofCatalystsDirectedbyGeneticAlgorithmsinaPlug-BasedMicrofluidicDeviceTestedwithOxidationofMethanebyOxygenJasonE.Kreutz,AntonShukhaev,WenbinDu,SashaDruskin,,,OlafsDaugulis,*andRustemF.Ismagilov*DepartmentofChemistryandInstituteforBiophysicalDynamics,TheUniVersity
2、ofChicago,929East57thStreet,Chicago,Illinois60637,andDepartmentofChemistry,UniVersityofHouston,Houston,Texas77204-5003ReceivedNovember20,2009;E-mail:r-ismagilov@uchicago.edu;olafs@uh.eduAbstract:Thispaperusesmicrofluidicstoimplementgeneticalgorithms(GA)todiscovernewhomogeneouscatalystsusingtheo
3、xidationofmethanebymolecularoxygenasamodelsystem.TheparametersoftheGAwerethecatalyst,acocatalystcapableofusingmolecularoxygenastheterminaloxidant,andligandsthatcouldtunethecatalyticsystem.TheGArequiredrunninghundredsofreactionstodiscoverandoptimizecatalystsystemsofhighfitness,andmicrofluidicsena
4、bledthesenumerousreactionstoberuninparallel.Thesmallscaleandvolumesofmicrofluidicsoffersignificantsafetybenefits.Themicrofluidicsystemincludedmethodstoformdiversearraysofplugscontainingcatalysts,introducegaseousreagentsathighpressure,runreactionsinparallel,anddetectcatalystactivityusinganinsituind
5、icatorsystem.Platinum(II)wasidentifiedasanactivecatalyst,andiron(II)andthepolyoxometalateH5PMo10V2O40(POM-V2)wereidentifiedasactivecocatalysts.ThePt/FesystemwasfurtheroptimizedandcharacterizedusingNMRexperiments.Afteroptimization,turnovernumbersofapproximately50wereachievedwithapproximatelyequal
6、productionofmethanolandformicacid.ThePt/Fesystemdemonstratedthecompatibilityofironwiththeentirecatalyticcycle.ThisapproachofGA-guidedevolutionhasthepotentialtoacceleratediscoveryincatalysisandotherareaswhereexplorationofchemicalspaceisessential,includingoptimizationofmaterialsforhydrogenstorag
7、eandCO2captureandmodifications.Introductionthisprocessofoptimizationinvitro,byusingtheprinciplesofevolutiontoidentifysolutionstoproblemswhereacomplexThispaperdemonstratesamicrofluidicmethodthatutilizes1,5,6mixtureofparametersmakessystemat
