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Open-Cage Copper Complexes Modulate Coordination and Charge Transfer.

Eric FirestoneRichard J StaplesThomas W Hamann
Published in: Inorganic chemistry (2024)
This study presents a novel copper-based redox shuttle that employs the PY5 pentadentate polypyridyl ligand in a dye-sensitized solar cell (DSSC). The [Cu(PY5)] 2+ complex exhibits a unique five-coordinate square pyramidal geometry, characterized by a strategically labile axial position, to facilitate efficient dye regeneration while minimizing electron recombination, thereby enhancing DSSC performance. Notably, the inclusion of 4- tert -butylpyridine (TBP) as an additive is shown to significantly modulate the electrochemical and photophysical properties of the copper complexes, attributed to its coordination to the vacant axial site. This interaction leads to an improved open-circuit voltage and overall device efficiency, with the complexes achieving promising efficiencies under standard solar irradiance. The findings underscore the potential of utilizing copper-based redox shuttles with designed ligand geometries to overcome the limitations of current DSSC materials, opening new avenues for the design and optimization of solar energy conversion devices. This work not only contributes to the fundamental understanding of the behavior of copper complexes in DSSCs but also paves the way for future research aimed at exploiting the full potential of such geometrical and electronic configurations for the development of more robust and efficient solar energy solutions.
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