DOI: https://doi.org/10.29363/nanoge.dynamic.2023.016
Publication date: 15th February 2023
Harnessing solar energy under diffuse light conditions is a challenge that can be addressed with photoelectrochemical cells (PECs). However, PECs suffer from efficiency losses due to electron-hole recombination. Inspired by natural photosynthesis, we demonstrate the use of supramolecular machinery with a pseudorotaxane topology as a strategy to inhibit recombination through an organization of molecular components that enables unbinding of the final electron acceptor upon reduction. We show that preorganization of a macrocyclic electron acceptor to a dye yields a pseudorotaxane that undergoes a fast (completed within ~50 ps) ‘ring launching’ event upon electron transfer from the dye to the macrocycle, releasing the anionic macrocycle and thus reducing charge recombination.. The PECs based on supramolecular machinery demonstrated a 16-fold and 5-fold increase in power conversion efficiency compared to devices featuring two control dyes that do not facilitate pseudorotaxane formation. This bio-inspired approach to integrate supramolecular machinery in PECs demonstrates the impact of molecular organization on the performance of devices for solar conversion technologies.
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