Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting

Fangwen Cheng, Olha Pavliuk, Steffen Hardt, Leigh Anna Hunt, Bin Cai, Tomas Kubart, Leif Hammarström, Nicolas Plumeré (), Gustav Berggren () and Haining Tian ()
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Fangwen Cheng: Uppsala University
Olha Pavliuk: Uppsala University
Steffen Hardt: Wilhelm-Johnen-Straße
Leigh Anna Hunt: Uppsala University
Bin Cai: Uppsala University
Tomas Kubart: Uppsala University
Leif Hammarström: Uppsala University
Nicolas Plumeré: Technical University of Munich
Gustav Berggren: Uppsala University
Haining Tian: Uppsala University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Dye-sensitized photoelectrodes consisting of photosensitizers and molecular catalysts with tunable structures and adjustable energy levels are attractive for low-cost and eco-friendly solar-assisted synthesis of energy rich products. Despite these advantages, dye-sensitized NiO photocathodes suffer from severe electron-hole recombination and facile molecule detachment, limiting photocurrent and stability in photoelectrochemical water-splitting devices. In this work, we develop an efficient and robust biohybrid dye-sensitized NiO photocathode, in which the intermolecular charge transfer is enhanced by a redox polymer. Owing to efficient assisted electron transfer from the dye to the catalyst, the biohybrid NiO photocathode showed a satisfactory photocurrent of 141±17 μA·cm−2 at neutral pH at 0 V versus reversible hydrogen electrode and a stable continuous output within 5 h. This photocathode is capable of driving overall water splitting in combination with a bismuth vanadate photoanode, showing distinguished solar-to-hydrogen efficiency among all reported water-splitting devices based on dye-sensitized photocathodes. These findings demonstrate the opportunity of building green biohybrid systems for artificial synthesis of solar fuels.

Date: 2024
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DOI: 10.1038/s41467-024-47517-9

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