Towards Long-Term Photostability of Solid-State Dye Sensitized Solar Cells

The solid‐state dye‐sensitized solar cell (DSSC) was introduced to overcome inherent manufacturing and instability issues of the electrolyte‐based DSSC and progress has been made to deliver high photovoltaic efficiencies at low cost. However, despite 15 years research and development, there still remains no clear demonstration of long‐term stability. Here, solid‐state DSSCs are subjected to the severe aging conditions of continuous illumination at an elevated temperature. A fast deterioration in performance is observed for devices encapsulated in the absence of oxygen. The photovoltaic performance recovers when re‐exposed to air. This reversible behavior is attributed to three related processes: i) the creation of light and oxygen sensitive electronic shunting paths between TiO2 and the top metal electrode, ii) increased recombination at the TiO2/organic interface, and iii) the creation of deep electron traps that reduce the photocurrent. The device deterioration is remedied by the formation of an insulating alumino‐silicate shell around the TiO2 nanocrystals, which reduces interfacial recombination, and the introduction of an insulating mesoporous SiO2 buffer layer between the top electrode and TiO2, which acts as a permanent insulating barrier between the TiO2 and the metal electrode, preventing shunting. Encapsulated solid‐state dye‐sensitized solar cells (ssDSSCs) show a reversible and quick deterioration in performance while aging under inert atmosphere. This is attributed to the activation of deep traps and the change in Schottky barrier at the TiO2 surface. This is remedied by forming an insulating alumino‐silicate “shell” around the TiO2 nanocrystals, and by introducing an insulating mesoporous SiO2 “buffer layer” between the top electrode and TiO2.