Publication date: 17th February 2025
Solar energy harvesting and conversion represent a compelling scientific, technological and societal to move away from the exploitation of fossil fuels. In this context, Dye-sensitized solar cells (DSSCs) are viable and cheap alternatives to conventional silicon-based cells with advantages in terms of transparency and efficiency in indoor conditions.[1] Ruthenium and polypyridine complexes holds the golden standard in this field, as they possess ideal characteristics such as long-lasting metal-ligand charge transfer (MLCT) states and efficient charge separation, limiting recombination at the dye-TiO2 interface. However, ruthenium is a rare and expensive metal, and the development of more sustainable energy devices based on earth-abundant metals is now a must. A quick glance at the periodic table reveals iron as a potential good candidate. However, striking photophysical differences exist between ruthenium(II) polypyridyl complexes and their Fe(II) analogues, the latter suffering from short-lived MLCT states resulting of their ultra-fast relaxation into metal-centered (MC) states. [2] Pyridyl-N-heterocyclic carbenes (pyridylNHC) brought a strong s-donor character required to promote a higher ligand field splitting of the iron d orbitals, resulting in a destabilization of the MC states over the MLCT manifold with slowdown of the excited state deactivation providing iron(II) complexes with tens of picoseconds lifetimes making them more promising for applications in DSSCs. [3] In this contribution I will present our recent advances in the development of photoactive iron-carbene dye sensitizers and characterization of iron-sensitized solar cells[4] with a focus on the computationally driven design of efficient sensitizers going from homoleptic to heteroleptic complexes (bearing different anchoring groups) and on electrolyte contents. Our synergistic computational and experimental approach led to the best photocurrent and efficiency ever reported for an iron sensitized solar cell (2% PCE and 9 mA/cm2) using a co-sensitization process.
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