氢化酶在生物技术中的应用,

26,266042NADPNADP1931StephensonSticklandEC1.12[12][NiFe][NiFeSe][Fe][NiFe]ThauerHmd[3]Hmd[FeS][Fe][NiFe]311H2H+1H2O31H2+1H2HO1H3H+1H2O31H2+1H3HO1H3H+2H2O32H2+1H2HO(2)p-H23o-H2(3)H232H++2e-12310X-[4][5]NADPH11(2Fd1mol4mol-.......-..-.......-..,201760192004-11-2927272005122ChemicalProductionandTechnology1mol0.37～3.3mol1940HansGaffron[6]ScenedesmusobliquusChlamydomonasreinhardtiiWuenschiers2ATPFdATPFdCO2[Fe]ⅡⅠⅡb6fI[7]Lee[8]O2O2O2AmaoDvulgarisCTABCTABThiocapsaroseopersicina2pH[9]nmolOhmiyaClostridiumparaputrificum[10～12]1.82[13][Fe][NiFe][NiFeSe][14]LaishelyBryant[15]DvulgarisHildenboroughFe2+[16]BergelRalstoniaeutrophaNAD[1718]NAD+316L[19](Fe3[PO4]28H2O)3NAD(H)NADP(H)[2021]NAD(P)H[22]PyrococcusfuriosusⅠPFH2ase28[23]NADPH2[24]6.2g/LNADPHTTN(1mol)1000001molPFH2aseⅠ10000molNADPHNADPHThermoanaerobiumsp.NADPHPFH2aseNADPHNADP+PFH2aseNADP+NADPH[25]2SS-99.5%1R2S-98%TTN100160NADP+/NADPH[2627][28]NADPH1.5～2hNADPHNADPHNADPH4CO2Karyakin[29]5[1]StephensonM,SticklandLH.Hydrogenaseabacterialenzymeactivatingmolecularhydrogen.[J].Thepropertiesofhydrogenase[J].Biochem1931,25205-214.[2]VignaisP,BilloudB,MeyerJ.Classificationandphylogenyofhydrogenases[J].FEMSMicrobiolRev2001,25455-501.[3]Lyonej,ShimaS,BuurmanG,etal.UV-A/blue-lightinactivationofthemetal-freehydrogenase(Hmd)frommethanogenicarchaea[J].EurJBiochem2004,(271)195-204.[4]DrennanCL,PetersJW.Surprisingcofactorsinmetalloenzymes[J].CurrOpinStructBiol2003,13220-226.[5]Albracht,SPJ.Mechanismofhydrogenactivation[J].BiochemPhysiolAnaerobicBacteria200320-34.[6]DelaceyAL,FermandezVM,RoussetM,etal.SpectroscopicandkineticcharacterizationofactivesitemutantsofdesulfovibriofructosovoransNi-Fehydrogenase[J].BiolInorgChem2003,8129-134.[7]ForesterS,SteinM,BrechtM,etal.SinglecrystalEPRstudiesofthereducedactivesiteof[NiFe]hydrogenasefromDesulfovibriovulgarisMiyazakiF[J].AmChemSoc2003,(125)83-93.[8]BrechtM,VanGasteliM,BuhrkeTetal.Directdetectionofahydrogenligandinthe[NiFe]centeroftheregulatoryH2-sensinghydrogenasefromRalstoniaeutrophainitsreducedstatebyHYSCOREandENDORspectroscopy[J].AmChemSoc2003,(125)13075-13083.[9]AmaoY,TomonouY,Okural.HighlyefficientphotochemicalhydrogenproductionsystemusingzincporphyrinandhydrogenaseinCTABmicellarsystem[J].SolarEnergyMaterSolarCells2003,79103-111.[10]LubitzW,BrechtM,FoersterSetal.EPRandENDORstudiesof[NiFe]hydrogenasecontributionstounderstandingthemechanismofbiologicalhydrogenconversion[J].ACSSymposiumSeries2003,(858)128-149.[11]SlepLD,NeeseF.Bioinorganicreactionmechanismsfromhigh-valentirontobioorganometallicchemistry[J].AngewChem.IntEdEngl2003,422942-2945.[12]VolbedaA,Fontecilla-CampsJC.TheactivesiteandcatalyticmechanismofNiFehydrogenases[J].DaltonTransactions20034030-4038.[13]EvansDJ,PickettCJ.Chemistryandthehydrogenases[J].ChemSocRev2003,32268-275.[14]MontetY,AmaraP,VolbedaAetalGasaccesstotheactivesiteofNi-FehydrogenasesprobedbyX-ray29292005122ChemicalProductionandTechnologycrystallographyandmoleculardynamics[J].NatStructBiol1997,4523-526.[15]NlcoletY,PirasC,LegrandPetal.DesulfovibriodesulfuricansironhydrogenasethestructureshowsunusualcoordinationtoanactivesiteFebinuclearcenter[J].Structure1999713-23.[16]ReismannS,HochleitnerE,WangHetal.TamingofapoisonbiosynthesisoftheNiFe-hydrogenasecyanideligands[J].Science2003,(299)1067-1070.[17]KesselDG.Globalwarming-facts,assessment,countermeasures[J].PetroleumScienceEng2000,26157-168.[18]EVANSJ.Powerofthepeople[J].ChemistryinBritain2000(3)30-33.[19]NandiR,SenguptaSMicrobialproductionofhydrogenanoverview[J].CritRevMicrobiol1998,2461-84.[20]DASilvaS,BassequvR,BERGELA.Electrontransferbetweenhydrogenaseand316Lstainlesssteelidentificationofahydrogenase-catalyzedcathodicreactioninanaerobicMIC[J].ElectroanalyticalChem2004,[561]93-102.[21]KaliaVC,LALS,GhalRetal.Mininggenomicdatabasestoidentifynovelhydrogenproducers[J].TrendsBiotechnol2003,21152-156.[22]HomannPH.Hydrogenmetabolismofgreenalgaediscoveryandearlyresearch-atributetoHansGaffronandhiscoworkers[J].PhotosynthRes2003,7693-103.[23]QianD-J,NakamuraC,WenkSetal.Electrochemicalhydrogenevolutionbyuseofaglassycarbonelectrodesandwichedwithclay,poly(butylviologen)andhydrogenase[J].MaterLett2003,(57)1130-1134.[24]GhirardiML,ZhangL,LEEJWetal.MicroalgaeagreensourceofrenewableH2[J].TrendsBiotechnol2000,18506-511.[25]ChardinB,GiiudicalticoniMT,DellucaG,GuigliarelliB.BruschiMHydrogenasesinsulfate-reducingbacteriafunctionaschromiumreductase[J].ApplMicrobiolBiotechnol2003,63315-321.[26]Michelc,Gludicl-OrticoniM-T,BaymannFetal.Bioremediationofchromatebysulfate-reducingbacteria,cytochromesandhydrogenases[J].Water,Air,SoilPollutionFocus2003,3161-169.[27]ValenliaCanteroE,Pena-CabriatesJJ,Martinez-RomeroE.Thecorrosioneffectsofsulfate-andferric-reducingbacterialconsortiaonsteel[J].Geomicrobiol2003,20157-169.[28]LaishleyEJ,BryantRD.Electronflowinferrousbiocorrosion[J].BiochemPhysiolAnaerobicBacteria2003252-260.[29]BenemannJ.Hydrogenbiotechnologyprogressandprospects[J].NatBiotechnol1996,141101-1103.2005350kt0&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&