Sensitizer Molecule Engineering - The Development Of Novel Ru(Ii

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1、SENSITIZERMOLECULEENGINEERING----------THEDEVELOPMENTOFNOVELRu(II)POLYPYRIDYLCOMPLEXESFORAPPLICATIONINDYESENSITIZEDSOLARCELLSYALISUNADissertationSubmittedtotheGraduateCollegeofBowlingGreenStateUniversityinpartialfulfillmentoftherequirementsforthedegreeofDOCTOROFPHILOSOPHYDecember,2009Committee:Dr.Fe

2、lixN.Castellano,AdvisorDr.WilliamK.IngleGraduateFaultyRepresentativeDr.MichaelY.OgawaDr.ThomasKinstle©2009YaliSunAllRightsReservediiiABSTRACTFelixN.Castellano,AdvisorThreeseriesofhydrophobicruthenium(II)polypyridylsensitizersforDSSCapplicationwiththemolecularstructureRu(N^N)(Hdcbpy)X2,+/2+2+[Ru(N^N^

3、N)(H2dcbpy)X]and[Ru(N^N)2(H2dcbpy)]weredesignedandsynthesizedinthisdissertation.Theirabsorptionmaximaandmolarextinctioncoefficientsweretunedwiththevariationofthecoordinatedpolypyridylligands.Fundamentalphotophysicalandelectrochemicalstudieswerecarriedoutbyusingabatteryofavailabletechniquesincludinga

4、bsorption,luminescencespectroscopy,lifetime,andcyclicanddifferentialpulsevoltammetrytoclarifytheeffectofligandelectronicstructureonphotophysicalpropertiesandredoxpropertiesofrelevantspectroscopicorbitalsofthesecomplexes.Initialphotovoltaicperformanceoftheirassociatedsolarcells,includingtheincidentph

5、otontocurrentefficiency(IPCE),theshortcircuitcurrentdensity(Isc),andtheopencircuitvoltage(Voc),wereevaluatedupon2514.5nmillumination(7.3W/m).Densityfunctionaltheory(DFT)calculationswerecarriedoutforthreeparticularsensitizerstoexploretherelationshipbetweenthephotovoltaicperformanceandthesensitizers’m

6、olecularstructure.Fromthecombinationofthetheoreticalandexperimentalapproaches,the“antenna”intheHOMO,suchas--NCSorCN,iscriticaltothedesignofsensitizersforefficientphotovoltaicperformanceinDSSCapplication.Regardlessoftheirstrongabsorptioninthevisibleregionofthespectrum,theRu(II)/pyrenechromophoresyiel

7、dlowsinglewavelengthconversionivefficiencyduetopostulatedcompetingintramolecularprocessessuchastripletenergytransfertopyrene.Amongtheselectedpromisingsensitizers,thesyntheticallyfacileheterolepticruth