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Direct Operando Visualization of Metal Support Interactions Induced by Hydrogen Spillover During CO2 Hydrogenation
Kellie Jenkinson1, Maria Chiara Spadaro2, Viktoria Golovanova3
1EMAT and NANOlab Center of Excellence, University of Antwerp, Antwerp, 2020, Belgium.
Understanding catalyst active sites is key for designing better catalysts. This study reveals how nickel nanoparticles on ceria promote active Ce3+ sites via hydrogen spillover, enhancing catalytic performance in reactions like CO2 hydrogenation.
Area of Science:
- Materials Science
- Catalysis
- Surface Chemistry
Background:
- Understanding catalyst active sites is crucial for rational catalyst design.
- Ce3+ sites and oxygen vacancies on ceria supports are vital for reactions like CO2 hydrogenation.
- Catalyst structures change under reaction conditions, necessitating operando characterization.
Purpose of the Study:
- To investigate temperature-induced changes in Ni nanoparticle-decorated mesoporous CeO2.
- To identify active catalyst states and structure-activity relationships under operando conditions.
- To elucidate the role of Ni-induced hydrogen spillover in active Ce3+ site formation.
Main Methods:
- In situ quantitative multimode electron tomography for morphological analysis.
- In situ heating electron energy loss spectroscopy for chemical characterization.
- Operando electron energy loss spectroscopy using a windowed gas cell.
Main Results:
- Observed temperature-induced morphological and chemical transformations in Ni/CeO2 catalysts.
- Identified Ni-induced hydrogen spillover as a key factor.
- Demonstrated enhanced catalytic performance linked to active Ce3+ site formation.
Conclusions:
- Ni nanoparticles promote active Ce3+ site formation on CeO2 through hydrogen spillover.
- Operando characterization is essential for understanding dynamic catalyst behavior.
- This work provides insights into designing advanced ceria-based catalysts.
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