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WenjunLuo* 俊
MyKeyLaboratoryofFlexibleElectronics(KLOFE)InstituteofAdvancedMaterials(IAM),NationalJiangsuSynergisticInnovationCenterforAdvancedMaterials(SICAM)NanjingTechUniversity(NanjingTech),Nanjing211816,China:
N.S.LewisNature414589SolarSolarconversionandstorageisonestepinaPECThefirstpaperonaPECcellforsolarwaterA.FujishimaandK.Honda,Nature238,37-38,Asinglephotoelectrodeforwatersplittingwithouta
Ap-ntandemPEC
EFH+.
SolarSolartohydrogenefficiency55PhotonPhotonflux(a
VB
PSI
n-photoanodep-Eg/e=1.23V+Vb(0.4V)+a(0.4V)+c(0.1V)+iRMurphyetal.Int.J.HydrogenEnergyMurphyetal.Int.J.HydrogenEnergy31,1999
-ntandemPECcellisthemostpromisingsystemwithhigh-efficiencyandlowcost
BiVO4和SuitablebandgapandHighabsorption3Highcarrier5.Low4.5.Low
270nmNaTaO3量子效A.Kudo,J.Am.Chem.Soc.125,3082,CBCBKudo,J.Am.Chem.Soc.121,11459,GaN-ZnO固溶體的量子效率和可見光分解水出氫K.Domen,Nature440,295,第一個具有可見光分解純水制氫的氧氮化
Nat.Mater.2009,8,
LiuetalJ.Am.Chem.Soc.2012,134,G.Liuetal,Angew.Chem.2013,125,
Powderede-EF (1)SeparatedH2andEasierHigherutilizationrateofAhalfPECNatureMaterials,10,434,電電催化劑Mo3S4使p‐Si光陰極出氫開啟電勢降低Naturematerials12,158,NatureMaterials,10,456,電流電流Cu2O光陰極在AM1.5下具有最大的PECperformanceofaFe2TiO5AtotalPECaGaInP2photocathode+1GaAsaGaInP2photocathode+1GaAs高高效分解水(>10%),但光穩(wěn)定性差,成本Naturephotonics6,824,Krol,NatureCommun.4,2195aWO3photoanode+1
aBiVO4photoanode+1SiaFe2O3photoanode+1DSSC
4photoanode+2Si
EnergyEnviron.Sci.4,4046Adv.Funct.Mater.22,3066Angew.Chem.Int.Ed.52,11016EnergyEnviron.Sci.6,347
EnergyEnviron.Sci.7,752Adv.EnergyMater.
Prof.
Prof.
DecreasingDecreasingReducing3.Suppressingback
Electronicstructuresandbandpositionsofsomevisible-light-responsephotoanodes2.1.1AnefficientBiVO4photoanodebydecreasing Bi(NO3)Bi(NO3)ionfor
Effectofions on
ClearMODClear
PhotocurrentPhotocurrent Driedat150oCWenjunLuoetal.EnergyEnviron.Sci.,2011,4,
PureTi4+NbOnlyMo6+,W6+canOnlyMo6+,W6+canenhancethephotocurrentof
PureSr2+Zn2+In3+La3+Ions inBiIncreasediffusiondistanceofphotogeneratedelectronsby
Effectof+6ions onCr6+impurityPhotocurrent/Photocurrent/mA22210
increasingdiffusiondistanceofincreasingdiffusiondistanceofphotogenerated,CarrierconcentrationincreasesafterMo
51/C51/C2(1010
Cr6+isdeepenergywhileMo6+orW6+isshallowZongyanZhao,WenjunLuoetal.Phys.Lett.A,374,2010,Differencebetweenshallowanddeeplevel
2.1.2.Decreasediffusiondistanceofphotogeneratedbymorphology
Donor
PhotocurrentPhotocurrent
ShallowenergylevelisbetterthandeepenergylevelPorousShallowenergylevelisbetterthandeepenergylevelXinZhao,WenjunLuo*etal.,Adv.EnergyMater. Whyaporousphotoelectrode
VisualizedevidenceforshorterholediffusiondistanceinaporousstructureCurrentCurrent
AbsorbanceAbsorbance 0
200
200IPCEIPCE
350400450500550600650ChargeSeperationChargeSeperation0380400420440460480500
380400420440460480500
200 200IPCEηsepIPCEηsepHigherlightHigherinterfacechargetransfer?200200500500Potential(V)vs.Amechanismforhigherperformanceinaporous
TorealizeefficientsolarseawatersplittingoutdoorsforfirstSolar(themostrenewableSolar(themostrenewable+Seawater(themostabundantnaturalresource)D D
WenjunLuoetal.EnergyEnviron.Sci.4,4046ZhigangZou,WenjunLuoetal.ChinesePatent, 2010,
11 Ld=20
Optimizationparticlesize<2Ld(40 ofsolarhydrogenproductionfromnaturalseawateroutdoors
RecordsolarphotocurrentofBiVO4photoanodesfromdifferentgroupsintheworldMyChoietal.,Chem.Soc.Rev.2.2.AnefficientTa3N5photoanodebyremoving
PreparationofTa3N5PhotonPhotonflux/mWcm
SolarSolartohydrogenefficiency/AM
OxidationandnitridationofTafoilsathigh
Why
550-
50
MingxueLi,WenjunLuo*etal.Angew.Chem.Int.Ed.2013,52,11016(insidebackcoverpaper) 4.8 umsolarenergyconversionMurphyetal.Int.J.HydrogenEnergy31,1999PhotocurrentafterthermalorPhotocurrentafterthermalormechanicalsurface1MNaOH,. Photocurrent/ Photocurrent/22
SurfaceSEMimagesof
3N5calcinedatdifferentSurfaceSurfacelayerisexfoliatedonthesampleat590oCorhigherduetointernal RoleofthesurfacePL EIS-570oC,withSEIntensity/570oC,withoutSElayer590oC,withoutIntensity/
-Z/Z/---
570oC,withSElayer570oCwithoutSElaer590oC,withoutSElayer610oC,withoutSE
0 20004000600080001000012000Z/ThedensityThedensityofthebinationcentersThesurfaceThesurfacepassivationlayerisathinlayerofTa3-xN5-yOy(<15nm)highOafterremovalofthesurfacepassivationMechanismofthephotocurrent
SolarwatersplittingafterCo(OH)x5.58TaN/Co(OH), 5TaNli5 TaN,3TaN/210 Potential/Vvs.(3.8mA/cm2Thesolarphotocurrentat1.23(3.8mA/cm2Thesolarphotocurrentat1.23VRHEis5.5mA/cm2,whichismuchhiherthantherecordvalueofthereviousTa3N5electrodeRecordsolarphotocurrentofusual
Amountofproducts/Amountofproducts/
Augustynski,J.Mater.Chem.18,2298(2008)
Gratzel,Angew.Chem.Int.Ed.49,64055.5
00
Time/
TheFaradaicefficienciesofH2andO2areabout85%and74%,respectively.Thephotocurrentmainlycomesfromwatersplitting,notTa3N5photo-corrosion.Choi,Science343,990Thephotocurrentmainlycomesfromwatersplitting,notTa3N5photo-corrosion.SurfacecorrosiononInGaNandFe2O3
PhotocurrentPhotocurrent.
-0.4-0.20.00.81.0
PurePure
×Potential(VMingxueLi,WenjunLuo,etal.Appl.Phys.Lett.2011,92,262110
MinglongZhang,WenjunLuo,etal.Electrochem.Comm.2012,23,41
DapengCao,WenjunLuo*etal.Energy Morphologiesbeforeandaftersurface
PLspectraandI-Vcurvesintheaba
Intensity/AftercorrosionIntensity/
DarkcurrentDarkcurrent
FTO-bubblewithO1 1
Potential/Vvs.
DarkcurrentofODarkcurrentofO2reductiondecreasesaftersurfaceShallowleveldo andmorphologycontrolcanreducebulkbinationandimprovePECperformance.Surfacesegregationoftenhappensduringpreparationofsamples,whichoftenplayaroleas binationcenters.Surfacepretreatmentcanimprovethephotoelectrochemcialperformance.ThisstrategyisuniversalandcanofferaguidancetoimprovePECperformanceofothermaterials.SuppressingbackreactioncanshiftthephotocurrentonsetpotentialofaFe2O3photoanodeandalsoimprovethePECperformance.Aftermodification,recordsolarphotocurrentinBiVO4andTa3N5photoanodeshavebeenobtained.Especially,anefficientBiVO4photoanodewasusedtosplitnaturalseawateroutdoorsforthefirstArtificialPhotosyntheticChemicalProcess2012-202115billionTheJointCenterforArtificialPhotosynthesis(JCAP)2010-2015Ananowirep-ntandemcellwith10timeshigherthan
ApowderphotocatalystsystemwithSTH10%in
KoreaCenterforArtificialPhotosynthesis(KCAP)APEC/PVcellwithSTH APEC/PVcellwithSTHPapersinNature/Science/Naturesister
OurgoalinaPECwatersplitting XinWen,WenjunLuo*etJ.Mater.Chem.A1,15479ShengHuang,WenjunLuo*etJ.Phys.D:Appl.Phys.46,ZhongjieGuan,WenjunLuo*etm16,2929AporousphotoanodeAporousAAporousp-ntandemPECcellwithSTH10%andlow-Toexplore‘Si-like’forsolarwatersplittingiskeyHighcarriermobilityHighstabilityLowSuitableHighcarriermobilityHighstabilityLow
Thi
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