Gas phase methanol synthesis for carbon-11 radiopharmaceuticals.pdf

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1、GASPHASEMETHANOLSYNTHESISFORCARBON-11RADIOPHARMACEUTICALSbyErikvanLierB.Eng.,McGillUniversity,May2001ATHESISSUBMITTEDINPARTIALFULFILLMENTOFTHEREQUIREMENTSFORTHEDEGREEOFMASTEROFAPPLIEDSCIENCEinTHEFACULTYOFGRADUATESTUDIES(ChemicalandBiologicalEngineering)THEUNIVERSITYOFBRITISHCOLUMBIAAugust2007©

2、ErikvanLier,2007AbstractCarbon-11radiopharmaceuticalsaregaininganincreasingimportanceinpositronemissiontomographyduetotheirimportanceindiagnosticmedicine.Themostwidespreadmethodofproductionoftheseradiopharmaceuticalsisbymethylationofanappropriateprecursorwiththehighlyreactive[nC]methyliodide.C

3、onventionalsynthesisofthisintermediateinvolvesliquidphasesynthesisof[nC]methanol,whichisthestepthatlimitsthespecificactivityofthefinalproduct.Acatalyticgasphasemethanolsynthesisprocesswaseval•uated,thatpromisestoavoidthelossofspecificactivity.Inthisprocedure,[nC]carbondioxideproducedinthetarge

4、tisfirsttrappedandpurified,thenconvertedto[nC]carbonmonoxideusingmolybdenumandfinallyreducedto[nC]methanolusingacopperzincoxidecatalystinthepresenceofhydrogen.Inthisstudyadevicetotrapandpurify[nC]carbondioxidewasdevelopedandopti•mized.[nC]Carbondioxideproducedintargetwasquantitativelytrappedat

5、-20°Conacarbonmolecularsievecolumnandquantitativelyreleasedinlessthan3.5minutes.Areactortoconvert50ppmcarbondioxidetocarbonmonoxide,basedonthereactionwithmolybdenum,wasdeveloped.Acommerciallyavailableprocesssimulatorwasusedtoassisttheoptimizationofoperatingconditionsandmolybdenumpretreatmentme

6、thods.Underoptimalconditions,carbondioxidewasconvertedtocarbonmonoxidewithover70%yield.Areactortocatalyticallyconvert50ppmcarbonmonoxidetomethanolwasdeveloped.Acopperzincoxidecatalystwaspreparedbyaco-precipitationmethod.Thecatalystwasiiactivatedbyreductionwithhydrogenandpassivatedwithcompresse

7、dairpriortomethanolsynthesis.Theeffectoftemperature,pressureandflowrateontheconversionofcarbonmonoxidetomethanolwerestudiedandresultswereusedtocreateakineticmodel.Thismodelwasusedtodetermineoptimaloperatingconditionsforthisreactorandpre