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Catalyst Initiation in the Oscillatory Carbonylation Reaction英文文献资料.doc

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Catalyst Initiation in the Oscillatory Carbonylation Reaction英文文献资料

HindawiPublishingCorporation InternationalJournalofChemicalEngineering Volume2011,ArticleID518592,11pages doi:10.1155/2011/518592 ResearchArticle CatalystInitiationintheOscillatoryCarbonylationReaction KatarinaNovakovicandJulieParker SchoolofChemicalEngineeringandAdvancedMaterials,NewcastleUniversity,NewcastleuponTyneNE17RU,UK CorrespondenceshouldbeaddressedtoKatarinaNovakovic,katarina.novakovic@ncl.ac.uk Received16March2011;Revised21April2011;Accepted26April2011 AcademicEditor:D.Yu.Murzin Copyright?2011K.NovakovicandJ.Parker.ThisisanopenaccessarticledistributedundertheCreativeCommonsAttribution License,whichpermitsunrestricteduse,distribution,andreproductioninanymedium,providedtheoriginalworkisproperly cited. Palladium(II)iodideisusedasacatalystinthephenylacetyleneoxidativecarbonylationreactionthathasdemonstratedoscillatory behaviourinbothpHandheatofreaction.Inanattempttoextractthereactionnetworkresponsiblefortheoscillatorynatureof thisreaction,thesystemwasdividedintosmallerpartsandtheywerestudied.Thispaperfocusesonunderstandingthereaction networkresponsiblefortheinitialreactionsofpalladium(II)iodidewithinthisoscillatoryreaction.Thespeciesresearchedinclude methanol,palladium(II)iodide,potassiumiodide,andcarbonmonoxide.Severalchemicalreactionswereconsideredandapplied inamodellingstudy.Thestudyrevealedthesigni?cantroleplayedbytracesofwatercontainedinthestandardHPLCgrade methanolused. 1.Introduction The aforementioned results imply the need for a fun- damental understanding of the PCPOC reaction in order to make use of the observed phenomena and apply the knowledge gained to other systems. The key to achieving thisisinobtainingareactionnetwork(i.e.,ratedetermining reactionsinachemicalmechanism)responsiblefortheoscil- latorynatureofthePCPOCreaction.ThePCPOCreaction systemoninitiationconsistsofsevenspecies:CH3OH,PdI2, KI, NaOAc, CO, Air, and C8H6. Conducting mechanistic modelling studies is di?cult due to the large number of species. In this work, a strategy that redu