Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction
Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evoluti...
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| Published in | Nature communications Vol. 11; no. 1; pp. 1029 - 8 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
25.02.2020
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt–support interaction and more 5
d
density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H
2
SO
4
and 46 mV in 1.0 M NaOH at 10 mA cm
−2
, and long-term durability in wide-pH electrolytes.
Understanding the structural dynamics of single-atom site in electrochemical reactions is crucial for design of an efficient catalyst. Here, the authors develop highly active Pt single-atom electrocatalyst, and reveal the dynamic evolution of active sites by using operando synchrotron spectroscopy. |
|---|---|
| AbstractList | Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt–support interaction and more 5
d
density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H
2
SO
4
and 46 mV in 1.0 M NaOH at 10 mA cm
−2
, and long-term durability in wide-pH electrolytes.
Understanding the structural dynamics of single-atom site in electrochemical reactions is crucial for design of an efficient catalyst. Here, the authors develop highly active Pt single-atom electrocatalyst, and reveal the dynamic evolution of active sites by using operando synchrotron spectroscopy. Understanding the structural dynamics of single-atom site in electrochemical reactions is crucial for design of an efficient catalyst. Here, the authors develop highly active Pt single-atom electrocatalyst, and reveal the dynamic evolution of active sites by using operando synchrotron spectroscopy. Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt-support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H SO and 46 mV in 1.0 M NaOH at 10 mA cm , and long-term durability in wide-pH electrolytes. Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt–support interaction and more 5 d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H 2 SO 4 and 46 mV in 1.0 M NaOH at 10 mA cm −2 , and long-term durability in wide-pH electrolytes. Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt–support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H2SO4 and 46 mV in 1.0 M NaOH at 10 mA cm−2, and long-term durability in wide-pH electrolytes.Understanding the structural dynamics of single-atom site in electrochemical reactions is crucial for design of an efficient catalyst. Here, the authors develop highly active Pt single-atom electrocatalyst, and reveal the dynamic evolution of active sites by using operando synchrotron spectroscopy. Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt-support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H2SO4 and 46 mV in 1.0 M NaOH at 10 mA cm-2, and long-term durability in wide-pH electrolytes.Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt-support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H2SO4 and 46 mV in 1.0 M NaOH at 10 mA cm-2, and long-term durability in wide-pH electrolytes. |
| ArticleNumber | 1029 |
| Author | Wang, Danhao Liu, Xiaokang Liu, Wei Wei, Shiqiang Zhang, Wei Fang, Shi Gu, Jian Zhu, Xiaorong Lin, Yue Li, Yafei Yao, Tao Lu, Junling |
| Author_xml | – sequence: 1 givenname: Shi orcidid: 0000-0001-9255-1579 surname: Fang fullname: Fang, Shi organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 2 givenname: Xiaorong surname: Zhu fullname: Zhu, Xiaorong organization: Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University – sequence: 3 givenname: Xiaokang surname: Liu fullname: Liu, Xiaokang organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 4 givenname: Jian surname: Gu fullname: Gu, Jian organization: Department of Chemical Physics, University of Science and Technology of China – sequence: 5 givenname: Wei orcidid: 0000-0002-6665-220X surname: Liu fullname: Liu, Wei organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 6 givenname: Danhao surname: Wang fullname: Wang, Danhao organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 7 givenname: Wei surname: Zhang fullname: Zhang, Wei organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 8 givenname: Yue orcidid: 0000-0001-5333-511X surname: Lin fullname: Lin, Yue organization: Department of Chemical Physics, University of Science and Technology of China – sequence: 9 givenname: Junling orcidid: 0000-0002-2607-6869 surname: Lu fullname: Lu, Junling organization: Department of Chemical Physics, University of Science and Technology of China – sequence: 10 givenname: Shiqiang orcidid: 0000-0002-2052-1132 surname: Wei fullname: Wei, Shiqiang organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China – sequence: 11 givenname: Yafei surname: Li fullname: Li, Yafei organization: Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University – sequence: 12 givenname: Tao orcidid: 0000-0001-8699-8294 surname: Yao fullname: Yao, Tao email: yaot@ustc.edu.cn organization: National Synchrotron Radiation Laboratory, University of Science and Technology of China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/32098951$$D View this record in MEDLINE/PubMed |
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| Snippet | Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site... Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site... Understanding the structural dynamics of single-atom site in electrochemical reactions is crucial for design of an efficient catalyst. Here, the authors... |
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| SubjectTerms | 639/301/299/886 639/4077 639/638/77 Absorption spectroscopy Carbon sources Catalysts Dynamic structural analysis Electrochemistry Electrolytes Evolution Humanities and Social Sciences Hydrogen Hydrogen evolution reactions multidisciplinary Platinum Science Science (multidisciplinary) Selectivity Single atom catalysts Sodium hydroxide Spectrum analysis Substrates Sulfuric acid Synchrotron radiation X ray absorption X-ray absorption spectroscopy |
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| Title | Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction |
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