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Gas Phase Glycerol Valorization over Ceria Nanostructures with Well-Defined Morphologies
Louise R Smith1, Mala A Sainna1, Mark Douthwaite1
1Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, U.K.
ACS Catalysis
|May 31, 2021
Summary
Catalyst morphology significantly impacts bio-renewable methanol production from glycerol. Polyhedral ceria catalysts yield substantially more methanol and hydroxyacetone compared to cubic ones, highlighting the importance of surface facets in catalyst design.
Area of Science:
- Catalysis
- Materials Science
- Renewable Energy
Background:
- Glycerol is a byproduct of biodiesel production, offering a potential source for bio-renewable chemicals.
- Developing efficient catalysts for glycerol valorization is crucial for sustainable chemical synthesis.
- Ceria (cerium oxide) is a versatile material with applications in catalysis.
Purpose of the Study:
- To investigate the relationship between ceria catalyst morphology and its surface facets on product distribution during glycerol vaporization and reaction.
- To optimize the yield of bio-renewable methanol from glycerol conversion.
- To understand the influence of catalyst structure on reaction pathways and intermediate formation.
Main Methods:
- Hydrothermal synthesis was employed to prepare ceria catalysts with distinct morphologies (cubic, rodlike, polyhedral).
- Glycerol solutions were vaporized and reacted over the synthesized ceria catalysts.
- Product distribution, including methanol and hydroxyacetone yields, was analyzed.
- Density functional theory (DFT) calculations were used to probe surface properties and reaction mechanisms.
Main Results:
- Cubic ceria catalysts exhibited low glycerol conversion, attributed to low surface area and high acidity.
- Polyhedral ceria catalysts achieved significantly higher methanol space-time-yields (201 g/h/kg at 400 °C) compared to cubic ones.
- Rodlike and polyhedral ceria showed a higher selectivity (ca. 45%) towards hydroxyacetone, a key intermediate, compared to cubic ceria (15%).
- DFT calculations suggested that the (100) surface of cubic ceria may be hydroxylated, limiting basic sites.
Conclusions:
- The exposed surface facets of ceria catalysts strongly influence product distribution and reaction pathways in glycerol conversion.
- Catalyst morphology is a critical factor for enhancing methanol and hydroxyacetone yields.
- Future catalyst design for bio-renewable chemical production should prioritize controlling surface facets for optimal performance.
