简介:Catalyticpropertiesofthemetal-organicframeworkCr-MIL-101insolvent-freecycloadditionofCO2toepoxidestoproducecycliccarbonatesusingtetrabutylammoniumbromideasco-catalysthavebeenexploredundermildreactionconditions(8barCO2,25C).Styreneandpropylenecarbonateswereformedwithhighyields(95%and82%,respectively).CatalyticperformanceofCr-MIL-101wascomparedwithotherMOFs:Fe-MIL-101,Zn-MOF-5andHKUST-1.Thecatalyticpropertiesofdifferentquaternaryammoniumbromides,Cr-MIL-101aswellasPW12/Cr-MIL-101compositematerialhavebeenassessedinoxidativecarboxylationofstyreneinthepresenceofbothtert-butylhydroperoxideandH2O2asoxidantsat8100barCO2and2580Cwithselectivitytostyrenecarbonateupto44%at57%substrateconversion.
简介:HierarchicalZSM-11microsphereswithintercrystallinemesoporouspropertiesandrod-likecrystalsintergrowthmorphologyhavebeensynthesizedusingaspotoftetrabutylammoniumasasingletemplate.XRD,FTIR,SEM,TEMandN2adsorptionanalysisrevealedthateachindividualparticlewascomposedofnanosizedrodcrystalsinsertingeachotherandtheintercrystallinevoidsexistingamongrodsgaveasignificantmesoporesizedistribution.Steamtreatmentresultdemonstratedtheexcellenthydrothermalstabilityofsamples.Variouscrystallizationmodesincludingconstanttemperaturecrystallization(one-stagecrystallization)andtwo-stagetemperature-varyingcrystallizationwithdifferent1ststagedurationswereinvestigated.TheresultssuggestedthatthecrystallizationmodesweremainlyresponsiblefortheadjustableparticlesizeandtexturalpropertiesofsampleswhilethesmallamountoftetrabutylammoniumbromidewasmainlyusedtodirecttheformationofbothZSM-11frameworkanditsintergrowthmorphology.Furthermore,theperformanceofoptimalZSM-11asanactivecomponentforthecatalyticpyrolysisofheavyoilwasalsoinvestigated.Comparedwiththecommercialpyrolysiscatalyst,thehierarchicalZSM-11catalystexhibitedahighselectivitytodesiredproducts(LPG+gasoline+diesel),aswellasamuchlowerdrygasandcokeyield,plusahighselectivityandyieldoflightolefins(C=3C=4)andverypoorselectivitytobenzene.Therefore,fullyopenmicropore-mesoporeconnectivitywouldmakesuchhierarchicallyporousZSM-11zeolitesveryattractiveforapplicationsincleanpetrochemicalcatalysisfield.
简介:Throughournewly-developed'chemicalvapordepositionintegratedprocess(CVD-IP)'usingcarbondioxide(CO2)astherawmaterialandonlycarbonsourceintroduced,CO2couldbecatalyticallyactivatedandconvertedtoanewsolid-formproduct,i.e.,carbonnanotubes(CO2-derived)ataquitehighyield(thesingle-passcarbonyieldinthesolid-formcarbon-productproducedfromCO2catalyticcaptureandconversionwasmorethan30%atasingle-passcarbon-base).Forcomparison,whenonlypurecarbondioxidewasintroducedusingtheconventionalCVDmethodwithoutintegratedprocess,nosolid-formcarbon-materialproductcouldbeformed.IntheadditionofsaturatedsteamatroomtemperatureinthefeedforCVD,thereweremuchmoreend-openingcarbonnano-tubesproduced,ataslightlyhighercarbonyield.Theseinspiringworksopenedaremarkableandalternativenewapproachforcarbondioxidecatalyticcapturetosolid-formproduct,comparingwiththatofCO2sequestration(CCS)orCO2mineralization(solidification),etc.Asaresult,therewasmuchlessbodyvolumeandalmostnogreenhouseeffectforthissolid-formcarbon-materialthanthoseofprimitivecarbondioxide.
简介:标题化合物(C30H35N3)以4-甲基苯甲醛、环十二酮和3-甲基-1-苯基-1H-吡唑-5-胺,在三氟乙酸和醋酸的作用下,经微波辐射合成得到.其结构通过单晶X射线衍射法确定,晶体属单斜晶系,空间群P21/c,相对分子质量Mr=437.61,晶胞参数a=1.08926(11)nm,b=2.1927(2)nm,c=1.04954(14)nm,V=2.4641(5)nm3,Z=4,晶胞密度Dc=1.180g/m3,吸收系数μ=0.069mm-1,单胞中电子的数目F(000)=944.晶体结构用直接法解出,经全矩阵最小二乘法对原子参数进行修正,最终的偏离因子为R=0.0468,ωR=0.0905.在晶体结构中新形成的吡啶环为共平面结构.