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Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis
Matteo Monai1, Kellie Jenkinson2, Angela E M Melcherts1
1Inorganic Chemistry and Catalysis Group, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, 3584 CG Utrecht, Netherlands.
Science (New York, N.Y.)
|May 11, 2023
Summary
Strong metal-support interactions (SMSI) on nickel/titanium dioxide catalysts are dynamic. Initial reduction and subsequent carbon dioxide hydrogenation reveal that SMSI overlayers can be removed or partially re-exposed, altering catalytic activity.
Area of Science:
- Catalysis
- Materials Science
- Surface Chemistry
Background:
- Reducible supports influence metal catalyst performance via strong metal-support interactions (SMSI), often involving suboxide overlayers.
- Understanding SMSI dynamics is crucial for designing efficient nanocatalysts.
Purpose of the Study:
- To investigate the dynamic behavior of TiOₓ overlayers on Ni/TiO₂ catalysts under reaction conditions.
- To elucidate the impact of SMSI on carbon dioxide hydrogenation and carbon-carbon coupling.
Main Methods:
- Operando electron microscopy
- Operando vibrational spectroscopy
- In situ studies of nickel/titanium dioxide catalysts
Main Results:
- Thin TiOₓ overlayers formed at 400°C reduction were fully removed during CO₂ hydrogenation.
- After 600°C reduction, CO₂ hydrogenation led to partial Ni re-exposure, creating Ni-TiOₓ interfacial sites.
- These interfacial sites favored carbon-carbon coupling by acting as a carbon species reservoir.
Conclusions:
- The study challenges static models of SMSI, revealing dynamic overlayer behavior.
- Partial re-exposure of metal sites at interfaces is key for specific catalytic reactions.
- Detailed, single-particle level operando studies are essential for accurate structure-activity relationship models.
