Is electron ping-pong limiting the catalytic hydrogen evolution activity in covalent photosensitizer-polyoxometalate dyads?

in: Chemical Communications (2020)
Dietzek, Benjamin; Luo, Yusen; Maloul, Salam; Wächtler, Maria; Winter, Andreas; Schubert, Ulrich S.; Streb, Carsten
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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