Is electron ping-pong limiting the catalytic hydrogen evolution activity in covalent photosensitizer–polyoxometalate dyads?†
Maria
Wächtler, 
ab
Andreas
Winter,
de
Ulrich S.
Schubert,
de
Carsten
Streb
*c
and
Benjamin
Dietzek
*abe
ab
Andreas
Winter,
de
Ulrich S.
Schubert,
de
Carsten
Streb
*c
and
Benjamin
Dietzek
*abe
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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