A Photosensitizer-polyoxometalate Dyad That Enables the Decoupling of Light and Dark Reactions for Delayed On-demand Solar Hydrogen Production

Overview

Journal Nat Chem

Specialty Chemistry

Date 2022 Jan 28

PMID 35087218

Authors

Sebastian Amthor

Sebastian Knoll

Magdalena Heiland

Linda Zedler

Chunyu Li

Djawed Nauroozi

Willi Tobaschus

Alexander K Mengele

Montaha Anjass

Ulrich S Schubert

Benjamin Dietzek-Ivansic

Sven Rau

Carsten Streb

Affiliations

Soon will be listed here.

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 H 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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