Charge transfer and storage during multi-electron redox processes are considered as key steps in various important chemical and biological conversions. However, for most photoresponsive devices, generation of high-energy and stable redox equivalents by light-excitation is usually difficult. Both the output energy and quantum yield of photocharges are limited. Besides the low quantum yield of photoexcited states and electrochemical constraints, other main limiting factors include the electronic conductivity, mechanical and photoelectrochemical stability of the electrode materials. Conductive polymers, such as polyaniline and poly (3,4-ethylenedioxyethiophene), are widely used in thin-film transistors and photovoltaics given their high conductivity, mechanical flexibility and stability. In this work, we prepared a series of photoresponsive polymer thin-film electrodes based on crosslinked hydrogels. The hydrogels were doped with small-molecular photosensitizers and electron mediators for photogeneration of stable and strong redox equivalents. Electrochemical and spectroscopic results show that the relatively high light-conversion efficiencies of the material originate from the balanced energetics between each component and the improved charge-transfer dynamics.

Photoresponsive polymer electrodes for generation of high-energy redox equivalents

ACS Spring Meeting 2021

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