An engineered photoelectrode for dye solar cells has been developed through the combination of three mesoporous stacks made of shape-tailored TiO 2 anatase nanocrystals, which have been ad hoc synthesized by suitable colloidal routes. Optimization of light harvesting and charge collection efficiency allowed us to obtain a high power conversion efficiency of 10.26%.Dye-sensitized solar cells (DSCs) are one of the most promising photovoltaic technologies for production of renewable, clean, and affordable energy.1 Among third-generation photovoltaic devices DSCs exhibit the highest performance; to date, a record power conversion efficiency (PCE) of 12.3% has been achieved with photoanodes consisting of 20 nm anatase TiO 2 nanocrystallites co-sensitized by YD2-o-C8 and Y123 dyes.
2As the crystal structure and geometry of the photoelectrode of a DSC are crucial to determining the photoelectrochemical properties of the system, various strategies have been pursued to conveniently engineer photoanodes with tailored features.
3-8Although a porous electrode made of nanocrystallites with a high internal surface area is essential to guarantee loading of large amounts of dye molecules, the diffusion of electrons is restricted by trapping and detrapping events along defects, surface states, and grain boundaries.9 A possible solution to improve the charge collection efficiency is the use of anisotropically shaped TiO 2 nanostructures, such as all-linear 10-14 or branched nanorods,
15-17nanowires 18,19 and nanotubes arrays, 20,21 which are able to provide extended directional pathways for rapid collection of photogenerated electrons. However, modest PCE values have been reported to date, mainly because of the reduced internal surface area offered by photoanodes which employ nanorods or nanowires with a mean size larger than 100 nm 12,22,23 and/or the severe degradation of the original structural-morphological features of the selected anisotropic TiO 2 nanocrystals upon sintering.
11,15,16Another versatile strategy to enhance the PCE is the implementation of relatively large nanoparticles (mean size > 400 nm) as scattering centers, which present a well-dened hierarchical nanostructure to ensure an acceptable value of effective surface area.24,25 However, photoanodes based on these nanomaterials hardly offer any further benets, such as, for instance efficient charge transport, because electron percolation within nanocrystallites is reasonably expected to be more difficult. Hence, there is still plenty of scope for the design and synthesis of materials which should simultaneously exhibit large surface areas for dye adsorption, efficient light scattering and fast electron transport.Herein we present an affordable and versatile approach to photoelectrode structuring by which the performance of a DSC can be maximised. Our strategy exploits a new class of hierarchically structured photoanodes consisting of different stacks of purposely selected anisotropically shaped TiO 2 nanocrystals which have been synthesized by advanced wet-che...