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1、1586Ind.Eng.Chem.Res.2004,43,1586-1590TunableSolventsforHomogeneousCatalystRecycleJieLu,²MichaelJ.Lazzaroni,²JasonP.Hallett,²AndreasS.Bommarius,²CharlesL.Liotta,³andCharlesA.Eckert,²SchoolofChemicalandBiomolecularEngineeringandSchoolofChemistryandBiochemistry
2、,GeorgiaInstituteofTechnology,Atlanta,Georgia30332-0100Anovelclassoftunablesolventsfacilitatesrecycleofhomogeneouscatalystsforbotheconomicandenvironmentaladvantages.Inamixedorganic-aqueoustunablesolvent(OATS),reactionsbetweenwater-solublecatalystsandmoderatel
3、yhydrophobicsubstratescanberunhomoge-neously,withsubsequentphaseseparationforproductpurificationandcatalystreuse.Oneexampledemonstratedisthedimethylether(DME)-watersystem,whichhasbeenemployedasabenignalternativetoorganicsolventsforalcoholdehydrogenase(ADH)-ca
4、talyzedreductionofhydrophobicketonescoupledwithregenerationofthecofactorNADH.WealsoshowthefeasibilityofabiphasicDME-waterseparationschemetocouplewiththebiocatalyticreaction.Thesubsequentdownstreamprocessingofferstheadvantagesofeasilyisolatingwater-insolublepr
5、oductsfromtheaqueousphaseandrecyclingenzyme-cofactor.OtherOATSsystemsarediscussedwherethepreferentialdissolutionofmodestpressuresofCO2causesphaseseparations,whichresultinverylargedistributioncoefficientsoftargetmoleculesinthebiphasicorganic-aqueoussystem,with
6、substantialpromiseastunablesolventsforbiocatalysis.Introductionproducthassufficientsolubilityinwater.Moreover,becauseenzymesaregenerallyexpensive,itiscommonHomogeneouscatalystsaregenerallymoreactiveandtoreusethemtoachieveturnovernumbersabove106.5moreselective
7、thanheterogeneouscatalysts,andfurtherAlso,thedifficultiesofdownstreamseparationand/ortheyprecludeanyneedformasstransportofreactantspurificationoftheproductandthelackofbiocatalystandproductstoandfromthesite.Theyareespeciallywithsuitablestability/activityinorga
8、nicsolutionsposeusefulforchiralsynthesisbecausetheyalmostalwaysasignificantchallengeforthecommercialproductionresultinsuperiorenantiomericexcesses.However,aofpromisingtherapeuticagents.Ab
