Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics
Abstract Photocatalytic hydrogen evolution efficiency is limited due to unfavorable carrier dynamics and thermodynamic performance. Here, we propose to introduce electronegative molecules to build an electric double layer (EDL) to generate a polarization field instead of the traditional built-in ele...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38600-8 |
| _version_ | 1797801387561582592 |
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| author | Chengxin Zhou Jian Gao Yunlong Deng Ming Wang Dan Li Chuan Xia |
| author_facet | Chengxin Zhou Jian Gao Yunlong Deng Ming Wang Dan Li Chuan Xia |
| author_sort | Chengxin Zhou |
| collection | DOAJ |
| description | Abstract Photocatalytic hydrogen evolution efficiency is limited due to unfavorable carrier dynamics and thermodynamic performance. Here, we propose to introduce electronegative molecules to build an electric double layer (EDL) to generate a polarization field instead of the traditional built-in electric field to improve carrier dynamics, and optimize the thermodynamics by regulating the chemical coordination of surface atoms. Based on theoretical simulation, we designed CuNi@EDL and applied it as the cocatalyst of semiconductor photocatalysts, finally achieved a hydrogen evolution rate of 249.6 mmol h−1 g−1 and remained stable after storing under environmental conditions for more than 300 days. The high H2 yield is mainly due to the perfect work function, Fermi level and Gibbs free energy of hydrogen adsorption, improved light absorption ability, enhanced electron transfer dynamics, decreased HER overpotential and effective carrier transfer channel arose by EDL. Here, our work opens up new perspectives for the design and optimization of photosystems. |
| first_indexed | 2024-03-13T04:49:42Z |
| format | Article |
| id | doaj.art-9dfdc22727504cde9654caf67d85712b |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T04:49:42Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-9dfdc22727504cde9654caf67d85712b2023-06-18T11:18:32ZengNature PortfolioNature Communications2041-17232023-06-0114111110.1038/s41467-023-38600-8Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamicsChengxin Zhou0Jian Gao1Yunlong Deng2Ming Wang3Dan Li4Chuan Xia5New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd.New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd.New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd.New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd.New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd.School of Materials and Energy, University of Electronic Science and Technology of ChinaAbstract Photocatalytic hydrogen evolution efficiency is limited due to unfavorable carrier dynamics and thermodynamic performance. Here, we propose to introduce electronegative molecules to build an electric double layer (EDL) to generate a polarization field instead of the traditional built-in electric field to improve carrier dynamics, and optimize the thermodynamics by regulating the chemical coordination of surface atoms. Based on theoretical simulation, we designed CuNi@EDL and applied it as the cocatalyst of semiconductor photocatalysts, finally achieved a hydrogen evolution rate of 249.6 mmol h−1 g−1 and remained stable after storing under environmental conditions for more than 300 days. The high H2 yield is mainly due to the perfect work function, Fermi level and Gibbs free energy of hydrogen adsorption, improved light absorption ability, enhanced electron transfer dynamics, decreased HER overpotential and effective carrier transfer channel arose by EDL. Here, our work opens up new perspectives for the design and optimization of photosystems.https://doi.org/10.1038/s41467-023-38600-8 |
| spellingShingle | Chengxin Zhou Jian Gao Yunlong Deng Ming Wang Dan Li Chuan Xia Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics Nature Communications |
| title | Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| title_full | Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| title_fullStr | Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| title_full_unstemmed | Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| title_short | Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| title_sort | electric double layer mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics |
| url | https://doi.org/10.1038/s41467-023-38600-8 |
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