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1、PublishedonWeb05/12/2006ElectrochemistryatSingle-WalledCarbonNanotubes:TheRoleofBandStructureandQuantumCapacitanceIddoHeller,JingKong,†KeithA.Williams,‡CeesDekker,andSergeG.Lemay*ContributionfromtheKaVliInstituteofNanoscience,DelftUniVersityofTechnology,L
2、orentzweg1,2628CJDelft,TheNetherlandsReceivedFebruary20,2006;E-mail:lemay@mb.tn.tudelft.nlAbstract:Wepresentatheoreticaldescriptionofthekineticsofelectrochemicalchargetransferatsingle-walledcarbonnanotube(SWNT)electrodes,explicitlytakingintoaccounttheSWNT
3、electronicbandstructure.SWNTshaveadistinctandlowdensityofelectronicstates(DOS),asexpressedbyasmallvalueofthequantumcapacitance.Weshowthatthisgreatlyaffectsthealignmentandoccupationofelectronicstatesinvoltammetricexperimentsandthustheelectrodekinetics.Wemo
4、delelectrochemistryatmetallicandsemiconductingSWNTsaswellasatgraphenebyapplyingtheGerischer-Marcusmodelofelectrontransferkinetics.WepredictthatthesemiconductingormetallicSWNTbandstructureanditsdistinctvanHovesingularitiescanberesolvedinvoltammetry,inamann
5、eranalogoustoscanningtunnelingspectroscopy.Consequently,SWNTsofdifferentatomicstructureyielddifferentrateconstantsduetostructure-dependentvariationsintheDOS.Interestingly,therateofchargetransferdoesnotnecessarilyvanishinthebandgapofasemiconductingSWNT,due
6、tosignificantcontributionsfromstateswhichareafewkBTawayfromtheFermilevel.ThecombinationofananometercriticaldimensionandthedistinctbandstructuremakesSWNTsamodelsystemforstudyingtheeffectoftheelectronicstructureoftheelectrodeonelectrochemicalchargetransfer.
7、IntroductiondemonstratedthatsemiconductingSWNTscanactaschannelsinnanoscaletransistors,allowingtheirconductancetobetunedCarboniswidelyusedaselectrodematerialforelectrochem-byelectrostaticinteractionwithasolid-stategate10oranistry.Thecombinationofawideusefu
8、lpotentialwindow,electrolytegate.11ApotentialappliedbetweenanSWNTandelectronicpropertiessimilartometals,anditsversatileorganicchemistrymakesp2carbonaspecialelectrodematerial.1theelectrolyteitisimmersedincanveryeffec
