RESEARCHARTICLE
alargevarietyofhigh-performance,low-cost,metal-freecatalystsforvariouspracticalenergydevices,particularlyinPEMfuelcells.
MATERIALSANDMETHODS
VA-NCNTwassynthesizedbypyrolysisofiron(II)phthalocyanineac-cordingtoourpreviouslypublishedprocedures(1).N-G-CNTcompositewassynthesizedbysequentiallycombiningamodifiedHummers’methodfortheGOfabrication(31),freeze-dryingamixtureofGOandoxidizedCNT,followedbyannealingat800°CinNHbefoundintheSupplementary3for3hours.ThepreparationdetailscanMaterials.ThetransitionmetalFe-derivedcontrolsample(Fe/N/C)wassynthesizedaccordingtoliteratures(11,46).Specifically,100mgofzeoliticimidazo-lateframeworks(ZIF8),togetherwith10mgoftris(1,10-phenanthroline)iron(II)perchlorateion,wasball-milledfor1hourandheatedinArat1000°Cfor1hourandthenat900°CunderNH3for15min.
TheelectrochemicalperformancesoftheaboveORRcatalystswerecharacterizedthrough(i)half-celltestsin0.1MKOHor0.1MHClO4electrolytesbyanRDEmethodand(ii)single-celltestswitha5-cm2MEAandpureHpressure.2/ODetailed2asfuelsat80°C,100%relativehumidity,and2-barbackelectrodefabricationandtestprocessesaredescribedintheSupplementaryMaterials.ThemorphologyandcompositioncharacterizationofthematerialsarealsogivenintheSup-plementaryMaterials.
SUPPLEMENTARYMATERIALS
Supplementarymaterialforthisarticleisavailableathttp://advances.sciencemag.org/cgi/content/full/1/1/e1400129/DC1
Fig.S1.CharacterizationofVA-NCNTs.
Fig.S2.ElectrocatalyticactivitiesoftheVA-NCNTcatalystinalkalineelectrolyte(O2-saturated0.1MKOH)byhalf-celltests.
Fig.S3.ElectrocatalyticactivitiesoftheVA-NCNTcatalystinacidicelectrolyte(O2-saturated0.1MHClO4)byhalf-celltests.
Fig.S4.Typicalcross-sectionSEMimagesoftheGDLwiththeMEAofVA-NCNTsasthecath-odecatalystlayer,Nafionmembrane(N211)astheseparator,andPt/Castheanode.Fig.S5.SEM(A)andTEM(B)imagesofN-CNTbundles.
Fig.S6.Typicalcross-sectionSEMimagesoftheGDLswiththeMEAsof(AtoC)N-G-CNT(2mgcm?2)and(DtoF)N-G-CNT+KB(0.5+2mgcm?2)asthecathodecatalystlayers,respectively.
Fig.S7.Tafelplot(A)andelectrontransfernumber(B)fortheN-G-CNTandPt/C(20%)asthefunctionofelectrodepotentialbyRRDEinoxygen-saturated0.1MKOHsolutionatascanspeedof5mVs?1andarotationspeedof1600rpm.
Fig.S8.Long-timestabilityandtolerancetomethanol/carbonmonoxideofmetal-freecatalystN-G-CNT.
Fig.S9.SEMimagesofcatalystlayercrosssectionsusedinRDEmeasurements.
Fig.S10.Electrocatalyticactivitiesofthecarbon-basedmetal-freeN-G-CNTcatalystsinacidicelectrolyte(O2-saturated0.1MHClO4)byhalf-celltests.
Fig.S11.Optimizationofcathodecatalystlayercomposition.
Fig.S12.Single-cellperformancecomparisonbetweenN-G-CNTandFe/N/Ccatalystsatthesamecatalystlayercomposition:catalyst(0.5mgcm?2)/KB(2mgcm?2)/Nafion(2.5mgcm?2).Fig.S13.PolarizationcurvesoftheN-G-CNTandindividualcomponentsofN-GorN-CNT.Fig.S14.Durabilityofthecatalystlayercomposedofmetal-freeN-G-CNT(2mgcm?2)+KB(2mgcm?2)inaPEMfuelcellmeasuredat0.5V.Fig.S15.Themetal-freecharacterofN-G-CNTcatalyst.
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Submitted20November2014Accepted24January2015Published27February201510.1126/sciadv.1400129
Citation:Shuietal.,N-dopedcarbonnanomaterialsaredurablecatalystsforoxygenreductionreactioninacidicfuelcells.Sci.Adv.1,e1400129(2015).
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Downloaded from http://advances.sciencemag.org/ on January 28, 2016N-doped carbon nanomaterials are durable catalysts foroxygen reduction reaction in acidic fuel cells
Jianglan Shui, Min Wang, Feng Du and Liming Dai (February 27,2015)
Sci Adv 2015, 1:.
doi: 10.1126/sciadv.1400129
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