Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes
Abstract Precise morphological control and identification of structure-property relationships pose formidable challenges for high-entropy alloys, severely limiting their rational design and application in multistep and tandem reactions. Herein, we report the synthesis of sub-nanometric high-entropy...
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| Formáid: | Alt |
| Teanga: | English |
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Nature Portfolio
2024-11-01
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| Sraith: | Nature Communications |
| Rochtain ar líne: | https://doi.org/10.1038/s41467-024-54589-0 |
| _version_ | 1826955460918378496 |
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| author | Yinghao Li Chun-Kuo Peng Yuntong Sun L. D. Nicole Sui Yu-Chung Chang San-Yuan Chen Yingtang Zhou Yan-Gu Lin Jong-Min Lee |
| author_facet | Yinghao Li Chun-Kuo Peng Yuntong Sun L. D. Nicole Sui Yu-Chung Chang San-Yuan Chen Yingtang Zhou Yan-Gu Lin Jong-Min Lee |
| author_sort | Yinghao Li |
| collection | DOAJ |
| description | Abstract Precise morphological control and identification of structure-property relationships pose formidable challenges for high-entropy alloys, severely limiting their rational design and application in multistep and tandem reactions. Herein, we report the synthesis of sub-nanometric high-entropy metallenes with up to eight metallic elements via a one-pot wet-chemical approach. The PdRhMoFeMn high-entropy metallenes exhibit high electrocatalytic hydrogen evolution performances with 6, 23, and 26 mV overpotentials at −10 mA cm−2 in acidic, neutral, and alkaline media, respectively, and high stability. The electrochemical measurements, theoretical simulations, and operando X-ray absorption spectroscopy reveal the actual active sites along with their dynamics and synergistic mechanisms in various electrolytes. Specially, Mn sites have strong binding affinity to hydroxyl groups, which enhances the water dissociation process at Pd sites with low energy barrier while Rh sites with optimal hydrogen adsorption free energy accelerate hydride coupling, thereby markedly boosting its intrinsic ability for hydrogen production. |
| first_indexed | 2025-02-17T23:52:04Z |
| format | Article |
| id | doaj.art-6aaf14e549cf461eb71d196eccc6c5ca |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2025-02-17T23:52:04Z |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-6aaf14e549cf461eb71d196eccc6c5ca2024-12-01T12:34:15ZengNature PortfolioNature Communications2041-17232024-11-0115111310.1038/s41467-024-54589-0Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenesYinghao Li0Chun-Kuo Peng1Yuntong Sun2L. D. Nicole Sui3Yu-Chung Chang4San-Yuan Chen5Yingtang Zhou6Yan-Gu Lin7Jong-Min Lee8School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang DriveDepartment of Material Science and Engineering, National Yang Ming Chiao Tung UniversitySchool of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang DriveSchool of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang DriveScientific Research Division, National Synchrotron Radiation Research CenterDepartment of Material Science and Engineering, National Yang Ming Chiao Tung UniversityZhejiang Key Laboratory of Petrochemical Environmental Pollution Control, Marine Science and Technology College, Zhejiang Ocean UniversityDepartment of Material Science and Engineering, National Yang Ming Chiao Tung UniversitySchool of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang DriveAbstract Precise morphological control and identification of structure-property relationships pose formidable challenges for high-entropy alloys, severely limiting their rational design and application in multistep and tandem reactions. Herein, we report the synthesis of sub-nanometric high-entropy metallenes with up to eight metallic elements via a one-pot wet-chemical approach. The PdRhMoFeMn high-entropy metallenes exhibit high electrocatalytic hydrogen evolution performances with 6, 23, and 26 mV overpotentials at −10 mA cm−2 in acidic, neutral, and alkaline media, respectively, and high stability. The electrochemical measurements, theoretical simulations, and operando X-ray absorption spectroscopy reveal the actual active sites along with their dynamics and synergistic mechanisms in various electrolytes. Specially, Mn sites have strong binding affinity to hydroxyl groups, which enhances the water dissociation process at Pd sites with low energy barrier while Rh sites with optimal hydrogen adsorption free energy accelerate hydride coupling, thereby markedly boosting its intrinsic ability for hydrogen production.https://doi.org/10.1038/s41467-024-54589-0 |
| spellingShingle | Yinghao Li Chun-Kuo Peng Yuntong Sun L. D. Nicole Sui Yu-Chung Chang San-Yuan Chen Yingtang Zhou Yan-Gu Lin Jong-Min Lee Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes Nature Communications |
| title | Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes |
| title_full | Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes |
| title_fullStr | Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes |
| title_full_unstemmed | Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes |
| title_short | Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes |
| title_sort | operando elucidation of hydrogen production mechanisms on sub nanometric high entropy metallenes |
| url | https://doi.org/10.1038/s41467-024-54589-0 |
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