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Reexploring Size-Dependent Catalytic Performance under Same Metal Loadings and Identifying Real Active Species: From
Jiankang Zhang1, Ye Ma2, Jiawen Yang3,4
1Interdisciplinary Research Center of Biology & Catalysis, School of Life Sciences, Northwestern Polytechnical University, Xi'an 710072, P. R. China.
Platinum (Pt) catalysts show increased activity with larger particle sizes, challenging previous assumptions. This study reveals nanoclusters and nanoparticles are the active sites for CO oxidation, offering insights into size-dependent catalysis.
Area of Science:
- Heterocatalysis
- Surface Science
- Materials Chemistry
Background:
- Size-dependent catalysis is crucial but complex, influenced by metal loading and support interactions.
- Research on size effects at identical metal loadings is scarce.
- Understanding particle size impact on catalytic activity is essential for catalyst design.
Purpose of the Study:
- To investigate size-dependent catalysis in platinum (Pt) catalysts with uniform metal loading.
- To elucidate the role of single atoms (SA), clusters, and nanoparticles in catalytic reactions.
- To explore the relationship between particle size, activity, and reaction mechanisms.
Main Methods:
- Synthesized SiO2-supported Pt catalysts with varying particle sizes (SA, cluster, nanoparticle) at 0.3 wt% loading using atomic layer deposition.
- Probed catalytic activity in CO oxidation reaction.
- Utilized in situ STEM, isotope labeling, and theoretical calculations to track dynamic processes and reaction mechanisms.
Main Results:
- Catalytic activity increased significantly with Pt particle size.
- Observed a gradual aggregation-activation process during CO oxidation.
- Pt nanoclusters/nanoparticles, not SAs, were identified as the active species.
- Achieved ultrahigh durability (>2160 h) attributed to dynamic size transformation and support confinement.
- Dissociation energy of small molecules correlated with particle size and activity.
Conclusions:
- Pt nanoclusters/nanoparticles are the primary active sites for CO oxidation, hydrogenation, and H2O2-involved reactions.
- Catalyst particle size is a critical descriptor for catalytic activity.
- Dynamic restructuring and support effects contribute to enhanced catalyst durability.
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