The nature of active sites in Pt-ReOx/Tio2 catalysts for selective hydrogenation of carboxylic acids to alcohols-中国Betway体育网页登陆

摘要 ThehighlydispersedPt–ReOX(x≤1)sitesca.0.5nminsizewereformedviaasuccessiveandstronginteractionoftheReprecursorwithtitaniaandthenofthePtcomplexwithdepositedlow-valentrheniumoxideclusters.Thesize,chargeandchemicalcompositionwerecharacterizedbymeansofHRTEM/STEMwithEDXmapping,XPS,andFTIRS.ThesesiteswithRe/Pt=2wereshowntobehighlyactiveandselectiveinthehydrogenationofcarboxylicacidtoalcoholunderverymildconditions(T=130°C,P=50bar).ThereactionrateconstantforthehydrogenationofhexanoicacidincreasedlinearlywiththePtcontent.Asforthehomogeneouspincer-typeRu-organiccomplexes,theactivePt–ReOXsitescandissociateheterolyticallythemolecularhydrogenwiththeformationofhydroxylgroupsandPthydrideforhydrogenationofthecarboxylicgroup.Indeed,TOFof20h-1andselectivityof98%–99%areapproachingthevaluestypicalofhomogeneouscatalysts.Thefirstorderkineticsdescribedwelltheexperimentaldataobtainedinawiderangeofreactionconditions.

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The nature of active sites in Pt-ReOx/Tio2 catalysts for selective hydrogenation of carboxylic acids to alcohols

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