Proceedings of 6th International Conference on Hybrid and Organic Photovoltaics (HOPV14)
Publication date: 1st March 2014
To realize solar cells and artificial photosynthesis on a large scale one should consider replacement of the efficient but rare Ru in photosensitizers (and catalysts). Fe is by far the best choice for the replacement of Ru because it is situated in the same group in the periodic table as Ru and because it is definitely abundant (6.2% of the Earth’s crust).
However, to use Fe in a photosensitizer transition-metal complex requires that the lifetime of the 3MLCT excited state is long enough to enable efficient utilization of the energy-rich electrons generated by light absorption in a solar cell or catalytic system. The lifetime of the 3MLCT-state in Fe-complexes so far available is intrinsically short, because of low-lying metal-centered (MC) 5T2 states to which the 3MLCT state decays on a femtosecond time scale. With the basic idea that a strongly σ-electron donating ligand should selectively destabilize (move to higher energy) the MC state by pushing electron density to the metal, we recently managed to increase the 3MLCT state lifetime by a factor of 100.1 This was achieved by attaching a strong s-donating ligand, a so-called N-heterocyclic carbene (NHC), to Fe(II) (Fig. 1). It should also be pointed out that only MLCT excited states (and not MC states) can drive the solar cell or photocatalytic processes since these states are localized on a ligand, which is the entity attaching a sensitizer to the electron acceptor metal oxide nanoparticle in a DSC, or the catalyst in a photocatalytic system. This results in fast and efficient electron transfer from the photosensitizer. In addition, only MLCT states have sufficiently high energy to drive the reactions.
Here we present the first successful attempt of utilizing strongly σ-donating NHC ligands to prolong the 3MLCT state of FeII complexes. The results of detailed ultrafast spectroscopy measurements of the excited state dynamics will be discussed. To the best of our knowledge, the observed 9 ps 3MLCT lifetime is the longest ever reported for any kind of Fe-based complex, and has been extended by almost two orders of magnitude compared to common [FeN6]2+. Notably, the structure of achieved complexes is amenable to further functionalization in the central py moiety in terms of electronic tuning and assembly construction.
Structure of our 1st generation Fe(NHC) complex.
Liu Y et al. Chem. Commun. 2013, 49, 6412
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