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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
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Understanding the Dynamic Aggregation in Single-Atom Catalysis.

Laihao Liu1, Tiankai Chen1, Zhongxin Chen1

  • 1School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, Guangdong, 518172, China.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|January 30, 2024
PubMed
Summary
This summary is machine-generated.

Single atoms in catalysts can dynamically aggregate into clusters, impacting performance. Understanding these dynamic changes is key to optimizing catalytic reactions.

Keywords:
catalyst stabilityoperando spectroscopiesreaction mechanismreversible aggregationsingle‐atom catalyststructural dynamism

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Area of Science:

  • Catalysis
  • Materials Science
  • Surface Chemistry

Background:

  • Single-atom catalysts (SACs) are crucial for molecular-level reaction understanding.
  • SACs can dynamically aggregate into clusters or nanoparticles under reactive conditions.
  • This aggregation is driven by thermodynamic or kinetic factors.

Purpose of the Study:

  • To uncover mechanistic nuances governing single-atom dynamic aggregation during reactions.
  • To explore factors influencing aggregation: intrinsic stability, migration barriers, external stimuli, and support effects.
  • To highlight cases where in situ formed clusters enhance catalytic performance.

Main Methods:

  • Theoretical analysis of intrinsic stability and site-migration barriers.
  • Investigation of external stimuli effects (temperature, voltage, adsorbates).
  • Consideration of catalyst support influence on dynamic behavior.

Main Results:

  • Dynamic aggregation can be beneficial or detrimental to catalytic performance.
  • In situ formed clusters, not initial single atoms, can be the active sites for improved catalysis.
  • Operando techniques are essential for understanding structural evolution.

Conclusions:

  • Controlling single-atom dynamic aggregation is vital for catalyst design.
  • Strategies like confinement and defect-engineering can regulate aggregation.
  • Further research using operando methods is needed to fully understand and control SAC dynamics.