Abstract
Given the limitations of the materials available for photoelectrochemical water splitting, a multiphoton (tandem) approach is required to convert solar energy into hydrogen efficiently and durably. Here we investigate a promising system consisting of a hematite photoanode in combination with dye-sensitized solar cells with newly developed organic dyes, such as the squaraine dye, which permit new configurations of this tandem system. Three configurations were investigated: two side-by-side dye cells behind a semitransparent hematite photoanode, two semitransparent dye sensitized solar cells (DSCs) in front of the hematite, and a trilevel hematite/DSC/DSC architecture. Based on the current-voltage curves of state-of-the-art devices made in our laboratories, we found the trilevel tandem architecture (hematite/SQ1 dye/N749 dye) produces the highest operating current density and thus the highest expected solar-to-hydrogen efficiency (1.36% compared with 1.16% with the standard back DSC case and 0.76% for the front DSC case). Further investigation into the wavelength-dependent quantum efficiency of each component revealed that in each case photons lost as a result of scattering and reflection reduce the performance from the expected 3.3% based on the nanostructured hematite photoanodes. We further suggest avenues for the improvement of each configuration from both the DSC and the photoanode parts.