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Issue 10, 2020
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Mesoporous silica-encapsulated gold core–shell nanoparticles for active solvent-free benzyl alcohol oxidation

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Abstract

Silica-encapsulated gold core@shell nanoparticles (Au@SiO2 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@SiO2 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@SiO2 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.

Graphical abstract: Mesoporous silica-encapsulated gold core–shell nanoparticles for active solvent-free benzyl alcohol oxidation

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Article information


Submitted
18 May 2020
Accepted
18 Aug 2020
First published
18 Aug 2020

React. Chem. Eng., 2020,5, 1939-1949
Article type
Paper

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

E. Hammond-Pereira, K. Bryant, T. R. Graham, C. Yang, S. Mergelsberg, D. Wu and S. R. Saunders, React. Chem. Eng., 2020, 5, 1939
DOI: 10.1039/D0RE00198H

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