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Cobalt Electrolyte/Dye Interactions in Dye-Sensitized Solar Cells: A Combined Computational and Experimental Study

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    Cobalt Electrolyte/Dye Interactions in Dye-Sensitized Solar Cells: A Combined Computational and Experimental Study
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    † Computational Laboratory for Hybrid and Organic Photovoltaics, Istituto CNR di Scienze e Tecnologie Molecolari, via Elce di Sotto 8, 06123 Perugia, Italy
    ‡ Laboratory for Photonics and Interfaces, Institution of Chemical Sciences and Engineering, School of Basic Sciences, Swiss Federal Institute of Technology, CH-1015 Lausanne, Switzerland
    § Instituto de Ciencia Molecular Parque Científico, Universidad de Valencia, C/José Beltrán, 2 46980 Paterna (Valencia), Spain
    ⊥ Dipartimento di Chimica, Università degli Studi di Perugia, via Elce di Sotto 8, 06123 Perugia, Italy
    [email protected]
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    Cite this: J. Am. Chem. Soc. 2012, 134, 47, 19438–19453
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    https://doi.org/10.1021/ja3079016
    Published October 31, 2012
    Copyright © 2012 American Chemical Society
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    Abstract

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    We report a combined experimental and computational investigation to understand the nature of the interactions between cobalt redox mediators and TiO2 surfaces sensitized by ruthenium and organic dyes, and their impact on the performance of the corresponding dye-sensitized solar cells (DSSCs). We focus on different ruthenium dyes and fully organic dyes, to understand the dramatic loss of efficiency observed for the prototype Ru(II) N719 dye in conjunction with cobalt electrolytes. Both N719- and Z907-based DSSCs showed an increased lifetime in iodine-based electrolyte compared to the cobalt-based redox shuttle, while the organic D21L6 and D25L6 dyes, endowed with long alkoxy chains, show no significant change in the electron lifetime regardless of employed electrolyte and deliver a high photovoltaic efficiency of 6.5% with a cobalt electrolyte. Ab initio molecular dynamics simulations show the formation of a complex between the cobalt electrolyte and the surface-adsorbed ruthenium dye, which brings the [Co(bpy)3]3+ species into contact with the TiO2 surface. This translates into a high probability of intercepting TiO2-injected electrons by the oxidized [Co(bpy)3]3+ species, lying close to the N719-sensitized TiO2 surface. Investigation of the dye regeneration mechanism by the cobalt electrolyte in the Marcus theory framework led to substantially different reorganization energies for the high-spin (HS) and low-spin (LS) reaction pathways. Our calculated reorganization energies for the LS pathways are in excellent agreement with recent data for a series of cobalt complexes, lending support to the proposed regeneration pathway. Finally, we systematically investigate a series of Co(II)/Co(III) complexes to gauge the impact of ligand substitution and of metal coordination (tris-bidentate vs bis-tridentate) on the HS/LS energy difference and reorganization energies. Our results allow us to trace structure/property relations required for further development of cobalt electrolytes for DSSCs.

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    Molecular orbitals, dye reorganization energies, optimized geometries, and NMR spectra. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: J. Am. Chem. Soc. 2012, 134, 47, 19438–19453
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