Using Supramolecular Machinery to Enhance the Efficiency of Photoelectrochemical Cells
Tessel Bouwens b
a Yusuf Hamied Department of Chemistry, University of Cambridge; Lensfield Road, Cambridge, UK
b Van ’t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands.
Proceedings of Dynamic Materials, Crystals and Phenomena Conference (DynaMIC23)
Fribourg, Switzerland, 2023 March 22nd - 24th
Organizers: Jovana Milic and Simon Krause
Invited Speaker, Tessel Bouwens, presentation 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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