CombinedEffectofNitrogen-andOxygen-ContainingFunctionaCombinedEffectofNitrogen-andOxygen-ContainingFunctionalGroupsofMicroporousActivatedCarbon.afm-journal.deEffectofNitrogen-andOxygen-ContainingGroupsofMicroporousActivatedCarbononElectrochemicalPerformanceinSupercapacitorsDenisaHulicova-Jurcakova,MykolaSeredych,GaoQingLu,andTeresastandingwhethermicroporesonly,[1–5]acombinationofmicroporesandmeso-pores,[6–9]ormesoporesonly[10–13]areopti-malforthemosteffectiveutilizationofthesurfaceareainadouble-layerformation.Chmiolaandco-workers[14–16]presentedadifferentviewofporeaccessibilitytoions.Theirresultsrevealedthattheporeswithawidthclosetothesizeofelectrosorbedions,i.e.,lessthan1nmfornon-aqueouselectro-lytes,arethemostactiveinadouble-layerformation.Thistheorywassupportedbyotherresearchgroups.[7,17]Inaddition,Huangetal.recentlyrevealedauniversaltheoreticalmodeltoexplainthechargestoragemechanismapplicabletodifferentporosity,carbonorigin,poresizedistribu-tionsandelectrolytes.[18,19]Thismodeltakestheporecurvatureintoaccount,incontra-dictionwiththetraditionalparallel-platecapacitor,anditappearsthatinthemicroporeregimesolvated/desolvatedionslineupalongtheporeaxistoformanelectricwire-in-cylindercapacitor,whileinthemesoporeregimetheyapproachtheporewalltoformanelectricdouble-cylindercapacitor.Theelec-tricdouble-layercapacitormodelbecomesapplicableinthemacroporeregionwheretheporecurvatureisnolongersignicant.Itshouldbenotedthatthismodelwassuccessfullyappliedtocarbonswithunimodalpores1.Introductionanddominantelectrosorptionofionsanditmaynotbeapplicableincarbonswithpseudocapacitiveenergystoragemechanism.Carbonelectrodematerialsforelectricdouble-layercapacitorsorTheseincludecarbonswithnitrogen-andoxygen-containingso-calledsupercapacitorshavebeenstudiedextensivelyinrecentsurfacegroups,whichhavebeeninvestigatedextensivelyinthelastyears.Oneofthemaininterestshasbeenfocusedonunder-decade.[20–26]Surfacegroupsintroducetheacid-basepropertiestocarbon[27–29]andgiverisetoFaradaicpseudocapacitivereac-[*]Prof.T.J.Bandosz,Dr.M.Seredychtions.[30]Pseudocapacitanceinnitrogen-enrichedcarbonshasTheCityCollegeofNewYork,DepartmentofChemistrybeenproposed,butnotconrmed,astheoxidation/reductionof160ConventAve,NewYork,NY10031(USA)negativelychargednitrogengroupslocatedattheperipheryofE-mail:tbandosz@ccny.cuny.edugraphene-likelayers.[22]Inthecaseofoxygenfunctionalities,theDr.D.Hulicova-Jurcakova,Prof.G.Q.Lumostdocumentedcaseisthereversibleoxidation/reductionofTheUniversityofQueenslandARCCentreofExcellenceforFunctionalNanomaterialshydroquinone/quinonegroups.[21,28,31]AustralianInstituteforBioengineeringandNanotechnologySinceoxygenfunctionalitiesarealwayspresentonthecarbonandSchoolofEngineeringsurfaceasaresultofactivationprocessesorasaresiduefromtheCornerCollegeandCooperRoads,StLucia,4072QLD(Australia)carbonsource,[32]thepseudocapacitivecontributiontothetotalcapacitanceofcarbonshouldbetakenintoaccount.Therefore,inDOI:10.1002/adfm.2021012364382021WILEY-VCHVerlagGmbHCo.KGaA,WeinheimAdv.Funct.Mater.2021,19,438–447CombinedEffectofNitrogen-andOxygen-ContainingFunctionalGroupsofMicroporousActivatedCarbon.afm-journal.deordertodevelopahigh-performancecarbonelectrodeforsupercapacitors,itiscrucialtounderstandthecombinedeffectofvarioustypesofcarbonsurfacefunctionalitiesandtheporestructureonitscapacitiveperformance.Tothebes...