Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
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 photocathode...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-47517-9 |
| _version_ | 1827284144451747840 |
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| author | Fangwen Cheng Olha Pavliuk Steffen Hardt Leigh Anna Hunt Bin Cai Tomas Kubart Leif Hammarström Nicolas Plumeré Gustav Berggren Haining Tian |
| author_facet | Fangwen Cheng Olha Pavliuk Steffen Hardt Leigh Anna Hunt Bin Cai Tomas Kubart Leif Hammarström Nicolas Plumeré Gustav Berggren Haining Tian |
| author_sort | Fangwen Cheng |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-04-24T09:50:56Z |
| format | Article |
| id | doaj.art-42d810dcc862464ca73d75a2dcd1085d |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-24T09:50:56Z |
| publishDate | 2024-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-42d810dcc862464ca73d75a2dcd1085d2024-04-14T11:22:44ZengNature PortfolioNature Communications2041-17232024-04-011511910.1038/s41467-024-47517-9Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splittingFangwen Cheng0Olha Pavliuk1Steffen Hardt2Leigh Anna Hunt3Bin Cai4Tomas Kubart5Leif Hammarström6Nicolas Plumeré7Gustav Berggren8Haining Tian9Department of Chemistry─Ångström laboratory, Physical Chemistry, Uppsala UniversityDepartment of Chemistry─Ångström laboratory, Molecular Biomimetics, Uppsala UniversityInstitute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, Wilhelm-Johnen-StraßeDepartment of Chemistry─Ångström laboratory, Physical Chemistry, Uppsala UniversityDepartment of Chemistry─Ångström laboratory, Physical Chemistry, Uppsala UniversityDepartment of Electrical Engineering, Solid-State Electronics, Uppsala UniversityDepartment of Chemistry─Ångström laboratory, Physical Chemistry, Uppsala UniversityTUM Campus Straubing for Biotechnology and Sustainability, Technical University of MunichDepartment of Chemistry─Ångström laboratory, Molecular Biomimetics, Uppsala UniversityDepartment of Chemistry─Ångström laboratory, Physical Chemistry, Uppsala UniversityAbstract 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.https://doi.org/10.1038/s41467-024-47517-9 |
| spellingShingle | Fangwen Cheng Olha Pavliuk Steffen Hardt Leigh Anna Hunt Bin Cai Tomas Kubart Leif Hammarström Nicolas Plumeré Gustav Berggren Haining Tian Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting Nature Communications |
| title | Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting |
| title_full | Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting |
| title_fullStr | Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting |
| title_full_unstemmed | Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting |
| title_short | Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting |
| title_sort | embedding biocatalysts in a redox polymer enhances the performance of dye sensitized photocathodes in bias free photoelectrochemical water splitting |
| url | https://doi.org/10.1038/s41467-024-47517-9 |
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