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Is electron ping-pong limiting the catalytic hydrogen evolution activity in covalent photosensitizer-polyoxometalate
Yusen Luo1, Salam Maloul2, Maria Wächtler1
1Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich-Schiller University Jena, Helmholtzweg 4, 07743 Jena, Germany and Department Functional Interfaces, Leibniz Institute of Photonic Technology (IPHT), Albert-Einstein-Strasse 9, 07745 Jena, Germany. benjamin.dietzek@leibniz-ipht.de.
Abstract:
Understanding the limitations of catalytic processes enables the design of optimized catalysts. Here, femtosecond transient absorption spectroelectrochemistry is used to explore the photophysics of polyoxometalate-based covalent photosensitizer-hydrogen evolution catalyst dyads. The study shows that the presence of light-driven forward and backward electron transfer, i.e. "electron ping-pong", is a limiting factor for charge accumulation on the polyoxometalate. Based on this insight, chemical means of optimizing catalyst performance are proposed.
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