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Updated: Jul 31, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Dynamic evolution of the active center driven by hemilabile coordination in Cu/CeO2 single-atom catalyst
Zheng Chen1, Zhangyun Liu1, Xin Xu2,3
1Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Key Laboratory of Computational Physical Sciences, Department of Chemistry, Fudan University, Shanghai, 200433, P. R. China.
Hemilability, a concept from homogeneous catalysis, is now shown to enhance heterogeneous single atom catalysts. Dynamic metal-support interactions tune active sites, boosting catalytic activity for reactions like CO oxidation.
Area of Science:
- Heterogeneous Catalysis
- Surface Science
- Computational Chemistry
Background:
- Hemilability describes reversible changes in metal-ligand coordination, crucial in homogeneous catalysis.
- This concept has been underexplored in heterogeneous catalysis, particularly for single atom catalysts.
Purpose of the Study:
- To investigate the influence of dynamic metal-support coordination on single atom catalyst electronic structure and activity.
- To extend the concept of hemilability to heterogeneous single atom catalysis.
Main Methods:
- Theoretical study using computational chemistry.
- Focus on CO oxidation reaction mechanism over substituted Cu1/CeO2 single atom catalysts.
Main Results:
- Dynamic evolution of metal-support coordination significantly alters the active center's electronic structure.
- Metal-adsorbate bonding strength is modulated throughout the reaction cycle (reactants to products).
- Catalyst activity is demonstrably increased due to these dynamic effects.
Conclusions:
- Hemilability effects can be extended to single atom heterogeneous catalysts.
- Active site dynamics play a critical role in catalysis.
- This concept offers new avenues for designing advanced single atom catalysts.
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