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processthatcouldlimitelectrochemicalreversibility.Ontheotherhand,thetendencyofNa+tonotadopttetrahedralcoordination(unlikeLi+)meansthattransitiontoaspinelstructureonpartialdesodiationfromNaMO2isnotfavoredasitisforsomeLiMO2compositionswhereitcauseslossofcapacityoncycling.Improvedcyclingstabilitycanbeattainedbyelementalsubstitutiontosuppressthephasetransitionsandreducevolumechanges.Theseremainashurdlestoovercomeforlong-termcyclelife.Fromapracticalpointofview,somesodiummetaloxidesexhibitahighsensitivitytomoisture,althoughO3phaseshavetheadvantageoffullsodiumcontent(meaninganonsodiatedanodecanbeused),andlessairsensitivity.Anothermajoradvanceistheveryrecentdiscoveryofsodium-based“high-voltage”layeredoxides,althoughitremainstobeseenwhethercyclingstabilitywillbeachievedinthisclassofmaterials.
ThelargersizeofNa+isalsoafactorforpolyanioncathodematerials,wheretheinfluenceofthealkalimetalsize/chargeratioissignificantindeterminingthethermody-namicallymoststablephase.Theseoftenhavenolithiumanalogue.Advanceshavebeenrealizedwithseveralnovel,excitingpolyanionmaterials:examplesincludeNa1.5VPO4.8F0.7and,mostrecently,Na2Fe2(SO4)3.ThelatterexhibitsaremarkablyhighFe3+/Fe2+redoxpotentialof3.8VversusNa,alongwithfastratekineticsthataresharedbytheformer.Althoughsulfateincreasestheredoxpotential,italsoconveysmoisturesensitivity:adisadvantagenotsharedbytherelativelymorestablephosphate-typematerials.Intriguingly,formanypolyanionmaterials,numerousmodelingstudieshaverevealedthattheactivationenergyforNa+ionhoppingisusuallylowerthanforLi+(becauseoflesspolarization),withvaluesbeingroutinelyaslowas0.3eV.Thisprovidesdistinctadvantagesforionmobility,thusexplainingthefastratekinetics.ThedevelopmentofnewuniquesodiumionpolyanionframeworktypeswillbepivotalfortheadvancementofthefieldofNaionbatteries.AsthechemistryofNaintercalationismuchlessadvancedthanitslithiumcounter-part,muchremainstobeexplored.Thisalsomeansover-comingthedisadvantageofthelargervolumeexpansion/contractionaffordedbythesodiumcationwithcleverdesignofsolid-statestructures.Wenotethatthischallengeiscommontobothsodiummetalpolyanionandlayeredmetaloxidesystems,butlesssoforthemoreopenPrussianblueframeworksolids,whichpresenttheirownspecialopportunities.
Newdevelopmentsinnegativeelectrodematerialsshowthatnotonlyhardcarbons,butgraphiticmaterialscanactasactiveNaionintercalationcompoundsatlowpotential.Muchscopeliesinthisarea.Sodiummetaldioxidesbasedontitaniumalsoshowmuchpromise.ItisalsoworthnotingthatbecauseNadoesnotalloywithaluminum(asdoesLi),thisallowsAlfoiltobeusedasacurrentcollectoratthenegativeelectroderatherthanCu.Thisisbeneficialintermsofbothcostandenergydensity.ThegenerallylowervoltageofNacompoundsalsoprovidesconsiderableadvantagesforthedevelopmentofthenegativeelectrode.Thepotentialofthesodium-containingpositiveelectrodeissimilarlylowered,thusprovidingopportunitiestoexplorematerialswherethelithiumanalogueshavetoohighapotentialtosupportmanyconventionalelectrolytes.
L.F.Nazaretal.
Overall,itisclearthatNaionbatteriescancompetewithLiionbatteriesinseveralimportantrespects,butthesodiumionbatteryisstillaveryimmaturetechnologyforenergystorageapplicationscomparedtoLiion.AsidefromtheNa/SandZEBRAhigh-temperaturesystems,nocommercializednon-aqueousNaionenergystoragebatteriesexistatpresent.Thereismuchopportunityforresearchanddevelopment.Manyinroadshavebeenmaderecentlyindevelopingnewpromisingpositiveelectrodematerials.Findinggoodnegativeelectrodematerialsremainsasignificantchallenge.Nonethe-less,compositionsencompassinglow-costtransitionmetalssuchasFe,Mn,andTiforeitherthepositiveornegativeelectrodesinNaionrechargeablebatterysystems,withoutsacrificinghighenergydensityandhighpower,arenowwithinscope.Thispaveswayforthediscoveryofnewsustainablecathodesmadewithearth-abundantelementsforlarge-scalebatteries.
Acknowledgements
ThisresearchwassupportedbytheNaturalSciencesandEngineeringCouncilofCanadathroughtheirDiscoveryandCanadaResearchChairprograms.L.F.N.gratefullyacknowl-edgestheirongoingsupportfornewelectrochemicaltechnol-ogies.
Received:October23,2014
Publishedonline:February4,2015
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