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Effect of Coordination Sphere Geometry of Copper Redox Mediators on Regeneration and Recombination Behavior in Dye-Sensitized Solar Cell Applications

  • Yasemin Saygili
    Yasemin Saygili
    Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • , 
  • Marko Stojanovic
    Marko Stojanovic
    Laboratory for Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • , 
  • Hannes Michaels
    Hannes Michaels
    Department of Chemistry—Ångström Laboratory, Uppsala University, 751 20 Uppsala, Sweden
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  • , 
  • Jan Tiepelt
    Jan Tiepelt
    Laboratory for Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • , 
  • Joel Teuscher
    Joel Teuscher
    Photochemical Dynamics Group, Ecole Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • , 
  • Arianna Massaro
    Arianna Massaro
    Department of Chemical Sciences, University of Naples Federico II, 80126 Naples, Italy
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  • Michele Pavone
    Michele Pavone
    Department of Chemical Sciences, University of Naples Federico II, 80126 Naples, Italy
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    Orcidhttp://orcid.org/0000-0001-7549-631X
  • , 
  • Fabrizio Giordano
    Fabrizio Giordano
    Laboratory for Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • Shaik M. Zakeeruddin
    Shaik M. Zakeeruddin
    Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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  • , 
  • Gerrit Boschloo
    Gerrit Boschloo
    Department of Chemistry—Ångström Laboratory, Uppsala University, 751 20 Uppsala, Sweden
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    Orcidhttp://orcid.org/0000-0002-8249-1469
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  • Jacques-E. Moser
    Jacques-E. Moser
    Photochemical Dynamics Group, Ecole Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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    Orcidhttp://orcid.org/0000-0003-0747-4666
  • , 
  • Michael Grätzel
    Michael Grätzel
    Laboratory for Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
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    Orcidhttp://orcid.org/0000-0002-0068-0195
  • , 
  • Ana B. Muñoz-García*
    Ana B. Muñoz-García
    Department of Physics “Ettore Pancini”, University of Naples Federico II, 80126 Naples, Italy
    *(A.B.M.-G.) E-mail:[email protected]
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  • Anders Hagfeldt*
    Anders Hagfeldt
    Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
    *(A.H.) E-mail: [email protected]
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  • Marina Freitag*
    Marina Freitag
    Department of Chemistry—Ångström Laboratory, Uppsala University, 751 20 Uppsala, Sweden
    *(M.F.) E-mail: [email protected]
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    Orcidhttp://orcid.org/0000-0002-4954-6851
Cite this: ACS Appl. Energy Mater. 2018, 1, 9, 4950–4962
Publication Date (Web):August 23, 2018
https://doi.org/10.1021/acsaem.8b00957
Copyright © 2018 American Chemical Society
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    Abstract

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    The recombination of injected electrons with oxidized redox species and regeneration behavior of copper redox mediators are investigated for four copper complexes, [Cu(dmby)2]2+/1+ (dmby = 6,6′-dimethyl-2,2′-bipyridine), [Cu(tmby)2]2+/1+ (tmby = 4,4′,6,6′- tetramethyl-2,2′-bipyridine), [Cu(eto)2]2+/1+ (eto = 4-ethoxy-6,6′-dimethyl-2,2′-bipyridine), and [Cu(dmp)2]2+/1+ (dmp = bis(2,9-dimethyl-1,10-phenantroline). These complexes were examined in conjunction with the D5, D35, and D45 sensitizers, having various degrees of blocking moieties. The experimental results were further supported by density functional theory calculations, showing that the low reorganization energies, λ, of tetra-coordinated Cu(I) species (λ = 0.31–0.34 eV) allow efficient regeneration of the oxidized dye at driving forces down to approximately 0.1 eV. The regeneration electron transfer reaction is in the Marcus normal regime. However, for Cu(II) species, the presence of 4-tert-butylpyridine (TBP) in electrolyte medium results in penta-coordinated complexes with altered charge recombination kinetics (λ = 1.23–1.40 eV). These higher reorganization energies lead to charge recombination in the Marcus normal regime instead of the Marcus inverted regime that could have been expected from the large driving force for electrons in the conduction band of TiO2 to react with Cu(II). Nevertheless, the recombination resistance and electron lifetime values were higher for the copper redox species compared to the reference cobalt redox mediator. The DSC devices employing D35 dye with [Cu(dmp)2]2+/1+ reached a record value for the open circuit voltage of 1.14 V without compromising the short circuit current density value. Even with the D5 dye, which lacks recombination preventing steric units, we reached 7.5% efficiency by employing [Cu(dmp)2]2+/1+ and [Cu(dmby)2]2+/1+ at AM 1.5G full sun illumination with open circuit voltage values as high as 1.13 V.

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