Designed Synthesis and Stacking Architecture of Solid and Mesoporous TiO₂ Nanoparticles for Enhancing the Light-Harvesting Efficiency of Dye-Sensitized Solar Cells

We fabricated solid and mesoporous TiO2 nanoparticles (NPs) with relatively large primary sizes of approximately 200 nm via inorganic templates for aero-sol-gel and subsequent aqueous-washing processes. The amount of dye molecules adsorbed by the internal pores in the mesoporous TiO2 NPs was increased by creating the nanopores within the solid TiO2 NPs. Simultaneously, the light-scattering effect of the mesoporous TiO2 NPs fabricated by this approach was secured by maintaining their spherical shape and relatively large average size. By precisely accumulating the fabricated solid or mesoporous 200 nm diameter TiO2 NPs on top of a conventional 25 nm diameter TiO2 NP-based underlayer, we could systematically examine the effect of the solid and mesoporous TiO2 NPs on the photovoltaic performance of dye-sensitized solar cells (DSSCs). Consequently, the stacking architecture of the mesoporous TiO2 NP-based overlayer, which functioned as both a light-scattering and dye-supporting medium, on top of a conventional solid TiO2 NP-based underlayer in a DSSC photoelectrode (i.e., double-layer structures) was found to be very promising for significantly improving the photovoltaic properties of conventional solid TiO2 NP single-layer-based DSSCs.