Multifunctional Polyoxometalate-Platforms for Supramolecular Light-driven Hydrogen Evolution

Autor: Carolin Müller, Alexander K. Mengele, Salam Maloul, Carsten Streb, Timo Jacob, Linda Zedler, Benjamin Dietzek-Ivanšić, Daniel Gaissmaier, Sven Rau, Matthias van den Borg
Rok vydání: 2021
Předmět:
DOI: 10.26434/chemrxiv-2021-d0fg9
Popis: Multifunctional supramolecular systems are a central research topic in light-driven solar energy conversion. Here, we report a polyoxometalate (POM)-based supramolecular dyad, where two platinum-complex hydrogen evolution catalysts are covalently anchored to an Anderson polyoxomolybdate anion. Supramolecular electrostatic coupling of the system to an iridium photosensitizer enables visible light-driven hydrogen evolution. Combined theory and experiment demon-strate the multifunctionality of the POM, which acts as photosensitizer / catalyst-binding-site and facilitates light-induced charge-transfer and catalytic turnover. Chemical modification of the Pt-catalyst site leads to increased hydrogen evolution reactivity. Mechanistic studies shed light on the role of the individual components and provide a molecular understanding of the interactions which govern stability and reactivity. The system could serve as a blueprint for multifunctional polyoxometalates in energy conversion and storage.
Databáze: OpenAIRE