Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

(整期优先)网络出版时间:2013-02-12
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Oxygen-andnitrogen-functionalizedcarbonnanotubes(OCNTsandNCNTs)wereappliedasmetal-freecatalystsinselectiveolefinhydrogenation.AseriesofNCNTswassynthesizedbyNH3post-treatmentofOCNTs.Temperature-programmeddesorption,N2physisorption,Ramanspectroscopy,high-resolutiontransmissionelectronmicroscopyandX-rayphotoelectronspectroscopywereemployedtocharacterizethesurfacepropertiesofOCNTsandNCNTs,aimingatadetailedanalysisofthetypeandamountofoxygenandnitrogen-containinggroupsaswellassurfacedefects.Thegas-phasetreatmentsappliedforoxygenandnitrogenfunctionalizationatelevatedtemperaturesupto600Cledtotheincreaseofsurfacedefects,butdidnotcausestructuraldamagesinthebulk.NCNTsshowedaclearlyhigheractivitythanthepristineCNTsandOCNTsinthehydrogenationof1,5-cyclooctadiene,andalsotheselectivitytocyclooctenewashigher.Thefavorablecatalyticpropertiesareascribedtothenitrogen-containingsurfacefunctionalgroupsaswellassurfacedefectsrelatedtonitrogenspecies.Incontrast,oxygen-containingsurfacegroupsandthesurfacedefectscausedbyoxygenspeciesdidnotshowclearcontributiontothehydrogenationcatalysis.