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Bozic-Weber, Biljana
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article
Understanding why replacing I3 -/I- by cobalt(II)/(III) electrolytes in bis(diimine)copper(I)-based dye-sensitized solar cells improves performance
Abstract
<p>The performances of dye-sensitized solar cells (DSCs) comprising heteroleptic bis(diimine)copper(I) based dyes combined with either [Co(bpy)<sub>3</sub>]<sup>2+/3+</sup>, [Co(phen)<sub>3</sub>]<sup>2+/3+</sup> or I3 <sup>-/I-</sup> redox mediators (bpy = 2,2′- bipyridine, phen = 1,10-phenanthroline) have been evaluated. The copper(I) dyes contain the anchoring ligand ((6,6′-dimethyl-[2,2′-bipyridine]-4,4′-diyl)bis(4,1-phenylene))bis(phosphonic acid), 1, and an ancillary ligand (2, 3 or 4) with a 2,9-dimethyl-1,10-phenanthroline metal-binding domain. Ligands 2 and 3 include imidazole 2′-functionalities with 4-(diphenylamino)phenyl (2) or 4-(bis(4-n-butoxy) phenylamino)phenyl (3) domains; in 4, the phen unit is substituted in the 4,7-positions with holetransporting 4-(diphenylamino)phenyl groups. The photoconversion efficiency, h, of each of [Cu(1)(2)]<sup>+</sup>, [Cu(1)(3)]<sup>+</sup> and [Cu(1)(4)] <sup>+</sup> considerably improves by replacing the I<sub>3</sub> <sup>-/I-</sup> electrolyte by [Co(bpy)<sub>3</sub>]<sup>2+/3+</sup> or [Co(phen)<sub>3</sub>]<sup>2+/3+</sup>, and after a change of electrolyte solvent (MeCN to 3-methoxypropionitrile). Due to the faster charge transfer kinetics and more positive redox potential, the cobalt-based electrolytes are superior to the I<sub>3</sub> <sup>-/I-</sup> electrolyte in terms of open-circuit voltage (V<sub>OC</sub>), short-circuit current (J<sub>SC</sub>) and η; values of V<sub>OC</sub> = 594 mV, J<sub>SC</sub> = 9.58 mA cm<sup>-2</sup> and η = 3.69% (relative to η = 7.12% for N719) are achieved for the best performing DSC which contains [Cu(1)(4)]<sup>+</sup> and [Co(bpy)<sub>3</sub>]<sup>2+/3+</sup>. Corresponding values for [Cu(1)(4)]<sup>+</sup> and I<sub>3</sub> <sup>-/I-</sup> DSCs are 570-580 mV, 5.98-6.37 mA cm<sup>-2</sup> and 2.43-2.62%. Electrochemical impedance spectroscopy (EIS) has been used to study DSCs with [Cu(1)(4)]<sup>+</sup> and the three electrolytes. EIS shows that the DSC with I<sub>3</sub> <sup>-/I-</sup> has the highest recombination resistance, whereas the [Co(phen)<sub>3</sub>]<sup>2+/3+</sup> electrolyte gives the highest chemical capacitance and V<sub>OC</sub> and, between [Co(bpy)<sub>3</sub>]<sup>2+/3+</sup> and [Co(phen)<sub>3</sub>]<sup>2+/3+</sup>, the higher recombination resistance. The [Co(phen)<sub>3</sub>]<sup>2+/3+</sup> electrolyte exhibits the highest mass transport restrictions which result in a lower J<sub>SC</sub> and D<sub>SC</sub> efficiency compared to the [Co(bpy)<sub>3</sub>]<sup>2+/3+</sup> electrolyte.</p>