Mesoporous silica-encapsulated gold core-shell nanoparticles for active solvent-free benzyl alcohol oxidation

Silica-encapsulated gold core@shell nanoparticles (Au@SiO 2 CSNPs) were synthesized via a tunable bottom-up procedure to catalyze the aerobic oxidation of benzyl alcohol. The nanoparticles exhibit a mesoporous shell which enhances selectivity by inhibiting the formation of larger species. Adding pot...

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Bibliographic Details
Published in:Reaction chemistry & engineering 2020-09, Vol.5 (1), p.1939-1949
Main Authors: Hammond-Pereira, Ellis, Bryant, Kristin, Graham, Trent R, Yang, Chen, Mergelsberg, Sebastian, Wu, Di, Saunders, Steven R
Format: Article
Language:English
Subjects:
Activation energy
Benzaldehyde
Benzyl alcohol
Catalysts
Chelating agents
Chelation
Conversion
Core-shell particles
Encapsulation
Gold
Nanoparticles
Oxidation
Pore size distribution
Porosity
Potassium carbonate
Selectivity
Silicon dioxide
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Summary:Silica-encapsulated gold core@shell nanoparticles (Au@SiO 2 CSNPs) were synthesized via a tunable bottom-up procedure to catalyze the aerobic oxidation of benzyl alcohol. The nanoparticles exhibit a mesoporous shell which enhances selectivity by inhibiting the formation of larger species. Adding potassium carbonate to the reaction increased conversion from 17.3 to 60.4% while decreasing selectivity from 98.4 to 75.0%. A gold nanoparticle control catalyst with a similar gold surface area took 6 times as long to reach the same conversion, achieving only 49.4% selectivity. These results suggest that the pore size distribution within the inert silica shell of Au@SiO 2 CSNPs inhibits the formation of undesired products to facilitate the selective oxidation of benzaldehyde despite a basic environment. A smaller activation energy, mass transport analysis, and mesopore distribution together suggest the Au@SiO 2 CSNP catalyst demonstrates higher activity through beneficial in-pore orientation, promoting a lower activation energy mechanistic pathway. Taken together, this is a promising catalytic structure to optimize oxidation chemistries, without leveraging surface-interacting factors like chelating agents or active support surfaces. Silica-encapsulated gold core@shell nanoparticles (Au@SiO 2 CSNPs) were synthesized via a tunable bottom-up procedure to catalyze the aerobic oxidation of benzyl alcohol.
ISSN:2058-9883
2058-9883
DOI:10.1039/d0re00198h