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. 2022 Mar;14(3):321-327.
doi: 10.1038/s41557-021-00850-8. Epub 2022 Jan 27.

A photosensitizer-polyoxometalate dyad that enables the decoupling of light and dark reactions for delayed on-demand solar hydrogen production

Sebastian Amthor  1 , Sebastian Knoll  1 , Magdalena Heiland  1 , Linda Zedler  2 , Chunyu Li  3 , Djawed Nauroozi  1 , Willi Tobaschus  4   5   6 , Alexander K Mengele  1 , Montaha Anjass  1   7 , Ulrich S Schubert  4   5   6 , Benjamin Dietzek-Ivanšić  8   9   10 , Sven Rau  11 , Carsten Streb  12   13
Affiliations

A photosensitizer-polyoxometalate dyad that enables the decoupling of light and dark reactions for delayed on-demand solar hydrogen production

Sebastian Amthor et al. Nat Chem. 2022 Mar.

Abstract

Decoupling the production of solar hydrogen from the diurnal cycle is a key challenge in solar energy conversion, the success of which could lead to sustainable energy schemes capable of delivering H2 independent of the time of day. Here, we report a fully integrated photochemical molecular dyad composed of a ruthenium-complex photosensitizer covalently linked to a Dawson polyoxometalate that acts as an electron-storage site and hydrogen-evolving catalyst. Visible-light irradiation of the system in solution leads to charge separation and electron storage on the polyoxometalate, effectively resulting in a liquid fuel. In contrast to related, earlier dyads, this system enables the harvesting, storage and delayed release of solar energy. On-demand hydrogen release is possible by adding a proton donor to the dyad solution. The system is a minimal molecular model for artificial photosynthesis and enables the spatial and temporal separation of light absorption, fuel storage and hydrogen release.

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