Combined Effect of Nitrogen- and Oxygen-Containing Functional Groups of Microporous Activated Carbon(2)

Combined Effect of Nitrogen- and Oxygen-Containing Functional Groups of Microporous Activated Carbon

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ordertodevelopahigh-performancecarbonelectrodeforsupercapacitors,itiscrucialtounderstandthecombinedeffectofvarioustypesofcarbonsurfacefunctionalitiesandtheporestructureonitscapacitiveperformance.Tothebestofourknowledge,thisimportantissuehasnotbeensystematicallyinvestigatedandnofundamentalunderstandingofpseudocapa-citancefromeitherthenitrogen-oroxygen-functionalgroupshasbeenreportedtodate.

Previouslywehaveinvestigatedaseriesofmicro/mesoporousactivatedcarbonenrichedwithnitrogen.[33]Verystrongdepen-denceofcapacitanceonthechemistryofsurfacegroupsaswellasontheporosityofcarbonswasobserved.Goodcorrelationswerefoundbetweenthenumberofbasicgroupsandthegravimetriccapacitance,andbetweenthenormalizedcapacitanceinmicro-poresandthedistributionofquaternaryandpyridinic-N-oxidenitrogenspeciesonthesurfaceofthemicropores,particularlyatheavyoperationregimes.Theconclusionwasthatthepseudo-capacitiveinteractionstakeplaceonnegativelychargedpyrrolic-Nandpyridinic-N,whilethepositivechargeonquaternary-Nandpyridinic-N-oxidehelpedinelectrontransferthroughthecarbon.Themicroporeswerethemosteffectiveinadouble-layerformationwhilemesoporesappearedtohavenopositiveeffectontheelectrochemicalperformance.

Inthispaperwestudythesynergisticeffectofnitrogen-andoxygen-containingsurfacefunctionalgroupsofsolelymicropor-ousactivatedcarbononitsperformanceina1MH2SO4supercapacitor.Detailedanalyzesofporestructureallowtheinvestigationofmosttheeffectiveporesforadouble-layerformationaswellasporesinwhichthepseudocapacitiveinteractionstakeplace.Accordingly,theresultsarediscussedintermsofnitrogentocarbonratio,nitrogenandoxygencontent,speci cchemicalarrangement,strengthofthesurfacefunctionalgroups,theirbasicityandthelocationofnitrogen-andoxygen-containinggroupsonthecarbonsurface.Theeffectofpore-sizedistributionandporestructureisanalyzedonthebasisofnitrogenandcarbondioxidesorption.

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