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Published on: July 18, 2017
In Situ High-Temperature Reaction-Induced Local Structural Dynamic Evolution of Single-Atom Pt on Oxide Support
Dongxu Yan1,2, Yanxia Gao1,2, Ming-Yu Qi3
1Xiamen Key Laboratory of Materials for Gaseous Pollutant Control, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China.
This study reveals how platinum single atoms (Pt1) activate during high-temperature alkane oxidation. An evolved Pt1-oxygen vacancy ensemble enhances catalyst activity, offering insights for designing efficient single-atom catalysts (SACs).
Area of Science:
- Heterogeneous Catalysis
- Materials Science
- Surface Chemistry
Background:
- Understanding active site evolution in single-atom catalysts (SACs) under reaction conditions is crucial for designing efficient catalysts.
- High-temperature reactions often lead to dynamic changes in catalyst structures, impacting performance.
- Platinum single atoms (Pt1) are promising for various catalytic applications, but their behavior under harsh conditions requires detailed investigation.
Purpose of the Study:
- To investigate the in situ activation and dynamic structural evolution of Pt single atoms (Pt1) during high-temperature light alkane oxidation.
- To elucidate the formation mechanism of active sites responsible for enhanced catalytic activity.
- To provide molecular-level insights into designing robust SACs for demanding applications.
Main Methods:
- In situ characterization of Pt single atoms (Pt1) during high-temperature reactions.
- Theoretical calculations (e.g., Density Functional Theory) to understand reaction mechanisms and active site formation.
- Analysis of the local coordination structure evolution under reaction conditions.
Main Results:
- The study demonstrates the in situ formation of a Pt1-oxygen vacancy (Pt1-OV) ensemble as the key active site during high-temperature alkane oxidation.
- Theoretical calculations confirm that lattice oxygen and dissociated H from methane form lattice hydroxyl, initiating Pt1-OV formation.
- Charge transfer from Pt1 and adjacent Mn to O-O bonds facilitates oxygen dissociation, boosting catalytic activity.
Conclusions:
- The in situ evolved Pt1-OV ensemble is an efficient and stable active site for high-temperature alkane oxidation.
- This work provides critical molecular-level understanding of reaction-induced structural evolution in SACs.
- The findings offer valuable guidance for designing high-performance SACs capable of operating under harsh reaction conditions.
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