Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction
Open accessAbstract
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.
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In-depth exploration of the real catalytic process and identification of active-site structure are rarely available due to structural remodeling, elemental valence changes and transformation of exposed active sites under realistic reaction conditions.
“the in-depth exploration of the real catalytic process and the identification of active-site structure are rarely available due to the structural remodeling, elemental valence changes and transformation of exposed active sites of electrocatalysts under realistic reaction conditions, probably resulting from additional electric potential, reaction temperature, or corrosive electrolyte36,37.”
From Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution (2022) · cites this paper as [37]
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Experimental — accuracy not yet measuredFor the benchmark catalyst Pt, the dependence of the intrinsic activity on the loading amount exhibits different behaviors in different domains approaching the single-atom limit.
“In fact, for the well-studied benchmark catalyst, Pt, the dependence of the intrinsic activity on the loading amount exhibits different behaviors in different domains approaching the single-atom limit.51”
From An energy-saving support made of silver nanowire aerogel for hydrogen evolution reaction (2023) · cites this paper as [51]
The Structural characterization section reports a Pt loading of about 2.5 wt% for the single-atom catalyst, and Electrochemical characterization reports higher intrinsic HER activity than for commercial 20% Pt/C. The paper does not establish how intrinsic activity depends on loading across different domains approaching the single-atom limit; it compares two catalysts rather than a loading series. No page numbers are available in our copy. (LLM, conf=0.78)
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- Authors
- Fang, S., Zhu, X., Liu, X., Gu, J., Liu, W., Wang, D., Zhang, W., Lin, Y., Lu, J., Wei, S., Li, Y., & Yao, T.
- Affiliations
- University of Science and Technology of China (CN)
- Nanjing Normal University (CN)
- Corresponding author
- Yao, Tao
- ORCID
- Venue
- Nature Communications
- Published
- 2020-02-25
- Volume
- 11
- Issue
- 1
- Pages
- 1029-1029
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC7042219
- OpenAlex
- W3008580165
- Cited by
- 585
- References
- 43
- Citations by year
- 2026: 51 · 2025: 77 · 2024: 96 · 2023: 109 · 2022: 121 · 2021: 99 · 2020: 32
- FWCI
- 17.83
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- Europe PMC (PubMed Central) (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- Salt Science Research Foundation (2017YFA0402800)
- National Natural Science Foundation of China (21533007, 11621063, 21471143, 2017YFA0402800)
- Youth Innovation Promotion Association of the Chinese Academy of Sciences (CX2310000091)
- National Synchrotron Radiation Laboratory
- Fundamental Research Funds for the Central Universities (11621063, WK2060030029, 2017YFA0402800, KY2310000020, WK2340000076)
- Youth Innovation Promotion Association
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- platinum single-atom catalysts, hydrogen evolution reaction, electrocatalysis, Pt-support interaction, nitrogen-doped carbon support, operando X-ray absorption spectroscopy, active site identification, overpotential, pH tolerance, catalyst stability
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