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1、ABSTRACTInthispaper,thereactionmechanismofacetylenehydrochlorinationinCu-basedcatalystwasstudiedusingthedensityfunctionaltheory(DFT).ThedeactivationmechanismofCu-basedcatalystandsomefactorswhichinfluencethereactionwerealsodiscussed.Theconclusionsderivedfromthisstudywouldclarifytheexperimentald
2、esignofnon-noblemetalcatalystwithhighperformance.ThecalculationresultsshowedthatthetwoCatomsofC2H2andCuatomformacompoundstructureviaaπ-σcoordinationbond.TheπelectronofC2H22+transferstotheunoccupiedmolecularorbitalofCu,thustheC≡Cbondisweaken.TheactivatedC2H2reactwiththecatalystandintermediatech
3、lorovinylisproduced.TheintermediateadsorbsHClontheCusite,theywillgeneratevinylchlorideandthecatalystrecoverstotheformerstructure.AsidereactionwouldbeoccurredviatheacetyleneadsorbedonthecatalystalonewhenthereisshortofHCl,theby-productofdichloroethylenewasformed.Therearetworeasonsforthedeactivat
4、ionofthecatalyst.Inthemainreaction,theintermediateisthecomplexstructurewithchlorovinylandcatalystwhichisreducedpartially,thedesorptionofchlorovinylandcatalystneedssomeenergy,sotheactivesiteofCucatalystwouldbeoccupiedandthecatalyticactivitywoulddecreaseifHClcan’tadsorbontheintermediate.Inthesid
5、ereaction,thecatalystisreducedtoelementalcopperandtheactivityislost.What’smore,theelectropositivityoftheactivesiteindifferentcoppersaltisdifferent,largertheelectropositivity,higherthecatalyticactivity.WhengraphenedopedwithNorP,thestructurebecomemorestablebecausetheelectronegativityoftheNatomis
6、high,andtheadsorptionenergybetweenthecatalystandgrapheneisamplified.ThereactionrateconstantsandtheactivationfreeenergycanalsobeinfluencedbyN/Pdoping.Thecatalystisamorphousonthesupporter,itwouldgeneratedifferentkindsofcluster,theatomicaveragebindingenergy,theatomicaverageadsorptionenergyandthec
7、hargeoftheatomareallrelatedwiththestructureofthecluster.The万方数据activitiesoftheclusterdecreasewiththenumberoftheatomsintheclusterbecausetherelativelylessatomicaveragecharge.KEYWORDS：DFT,acetylenehydrochlorination,Cu-basedcatalyst,reactio
