简介:Inthiswork,theinfluenceofCO2onthestructuralvariationandcatalyticperformanceofNa2WO4/Mn/SiO2foroxidativecouplingofmethanetoethylenewasinvestigated.ThecatalystwaspreparedbyimpregnationmethodandcharacterizedbyXRD,RamanandXPStechniques.AppropriateamountofCO2inthereactantgasesenhancedtheformationofsurfacetetrahedralNa2WO4speciesandpromotedthemigrationofOinMOx,Na,Wfromthecatalystbulktosurface,whichwerefavorableforoxidativecouplingofmethane.WhenthemolarratioofCH4/O2/CO2was3/1/2,enrichedsurfacetetrahedralNa2WO4speciesandhighsurfaceconcentrationofOinMOx,Na,Wweredetected,andthenhighCH4conversionof33.1%andhighC2H4selectivityof56.2%wereobtained.WithfurtherincreaseofCO2inthereagentgases,thecontentofactivesurfacetetrahedralNa2WO4speciesandsurfaceconcentrationofOinMOx,Na,Wdecreased,whilethatofinactivespecies(MnWO4andMn2O3)increaseddramatically,leadingtolowCH4conversionandlowC2H4selectivity.ItcouldbespeculatedthatNa2WO4crystalwastransformedintoMnWO4crystalwithexcessiveCO2addedunderthereactionconditions.PretreatmentofNa2WO4/Mn/SiO2catalystbymoderateamountofCO2beforeOCMalsopromotedtheformationofNa2WO4species.