Electrolytes Based on TEMPO–Co Tandem Redox Systems Outperform Single Redox Systems in Dye‐sensitized Solar Cells

A new TEMPO–Co tandem redox system with TEMPO and Co(bpy)(3) (2+/3+) has been investigated for the use in dye‐sensitized solar cells (DSSCs). A large open‐circuit voltage (V (OC)) increase, from 862 mV to 965 mV, was observed in the tandem redox system, while the short‐circuit current density (J (SC)) was maintained. The conversion efficiency was observed to increase from 7.1 % for cells containing the single Co(bpy)(3) (2+/3+) redox couple, to 8.4 % for cells containing the TEMPO–Co tandem redox system. The reason for the increase in V (OC) and overall efficiency is ascribed to the involvement of partial regeneration of the sensitizing dye molecules by TEMPO. This assumption can be verified through the observed much faster regeneration dynamics exhibited in the presence of the tandem system. Using the tandem redox system, the faster recombination problem of the single TEMPO redox couple is resolved and the mass‐transport of the metal‐complex‐based electrolyte is also improved. This TEMPO–Co tandem system is so far the most effienct tandem redox electrolyte reported not involving iodine. The current results show a promising future for tandem system as replacements for single redox systems in electrolytes for DSSCs.