Revealing operando surface defect–dependent electrocatalytic performance of Pt at the subparticle level Article Swipe
Yi Xiao
,
Zhichao Guo
,
Jing Cao
,
Ping Song
,
Bo Yang
,
Weilin Xu
·
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1073/pnas.2317205121
YOU?
·
· 2024
· Open Access
·
· DOI: https://doi.org/10.1073/pnas.2317205121
Understanding the operando defect–tuning performance of catalysts is critical to establish an accurate structure–activity relationship of a catalyst. Here, with the tool of single-molecule super-resolution fluorescence microscopy, by imaging intermediate CO formation/oxidation during the methanol oxidation reaction process on individual defective Pt nanotubes, we reveal that the fresh Pt ends with more defects are more active and anti-CO poisoning than fresh center areas with less defects, while such difference could be reversed after catalysis-induced step-by-step creation of more defects on the Pt surface. Further experimental results reveal an operando volcano relationship between the catalytic performance (activity and anti-CO ability) and the fine-tuned defect density. Systematic DFT calculations indicate that such an operando volcano relationship could be attributed to the defect-dependent transition state free energy and the accelerated surface reconstructing of defects or Pt-atom moving driven by the adsorption of the CO intermediate. These insights deepen our understanding to the operando defect–driven catalysis at single-molecule and subparticle level, which is able to help the design of highly efficient defect-based catalysts.
Related Topics
Concepts
Catalysis
Adsorption
Molecule
Density functional theory
Materials science
Chemical physics
Scanning tunneling microscope
Fluorescence
Atom (system on chip)
Nanotechnology
Photochemistry
Chemical engineering
Chemistry
Computational chemistry
Physical chemistry
Organic chemistry
Computer science
Embedded system
Quantum mechanics
Physics
Engineering
Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1073/pnas.2317205121
- OA Status
- green
- Cited By
- 10
- References
- 71
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4398197930
All OpenAlex metadata
Raw OpenAlex JSON
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https://openalex.org/W4398197930Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1073/pnas.2317205121Digital Object Identifier
- Title
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Revealing operando surface defect–dependent electrocatalytic performance of Pt at the subparticle levelWork title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2024Year of publication
- Publication date
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2024-05-22Full publication date if available
- Authors
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Yi Xiao, Zhichao Guo, Jing Cao, Ping Song, Bo Yang, Weilin XuList of authors in order
- Landing page
-
https://doi.org/10.1073/pnas.2317205121Publisher landing page
- Open access
-
YesWhether a free full text is available
- OA status
-
greenOpen access status per OpenAlex
- OA URL
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https://www.ncbi.nlm.nih.gov/pmc/articles/11145244Direct OA link when available
- Concepts
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Catalysis, Adsorption, Molecule, Density functional theory, Materials science, Chemical physics, Scanning tunneling microscope, Fluorescence, Atom (system on chip), Nanotechnology, Photochemistry, Chemical engineering, Chemistry, Computational chemistry, Physical chemistry, Organic chemistry, Computer science, Embedded system, Quantum mechanics, Physics, EngineeringTop concepts (fields/topics) attached by OpenAlex
- Cited by
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10Total citation count in OpenAlex
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2025: 10Per-year citation counts (last 5 years)
- References (count)
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71Number of works referenced by this work
- Related works (count)
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10Other works algorithmically related by OpenAlex
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