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Alumina-grafted SBA-15 as a high performance support for Pd-catalysed cinnamyl alcohol selective oxidation
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Parlett, Christopher M. A., Durndell, Lee J., Machado, Andreia, Cibin, Giannantonio, Bruce, Duncan W., Hondow, Nicole S., Wilson, Karen and Lee, Adam F. (2014) Alumina-grafted SBA-15 as a high performance support for Pd-catalysed cinnamyl alcohol selective oxidation. Catalysis Today, 229 . pp. 46-55. doi:10.1016/j.cattod.2013.11.056 ISSN 0920-5861.
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Official URL: http://dx.doi.org/10.1016/j.cattod.2013.11.056
Abstract
Ultrathin alumina monolayers grafted onto an ordered mesoporous SBA-15 silica framework afford a composite catalyst support with unique structural properties and surface chemistry. Palladium nanoparticles deposited onto Al-SBA-15 via wet impregnation exhibit the high dispersion and surface oxidation characteristic of pure aluminas, in conjunction with the high active site densities characteristic of thermally stable, high-area mesoporous silicas. This combination confers significant rate enhancements in the aerobic selective oxidation (selox) of cinnamyl alcohol over Pd/Al-SBA-15 compared to mesoporous alumina or silica supports. Operando, liquid-phase XAS highlights the interplay between dissolved oxygen and the oxidation state of palladium nanoparticles dispersed over Al-SBA-15 towards on-stream reduction: ambient pressures of flowing oxygen are sufficient to hinder palladium oxide reduction to metal, enabling a high selox activity to be maintained, whereas rapid PdO reduction and concomitant catalyst deactivation occurs under static oxygen. Selectivity to the desired cinnamaldehyde product mirrors these trends in activity, with flowing oxygen minimising Csingle bondO cleavage of the cinnamyl alcohol reactant to trans-β-methylstyrene, and of cinnamaldehyde decarbonylation to styrene.
Item Type: | Journal Article | ||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||
Journal or Publication Title: | Catalysis Today | ||||||
Publisher: | Elsevier BV | ||||||
ISSN: | 0920-5861 | ||||||
Official Date: | 15 June 2014 | ||||||
Dates: |
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Volume: | 229 | ||||||
Page Range: | pp. 46-55 | ||||||
DOI: | 10.1016/j.cattod.2013.11.056 | ||||||
Status: | Peer Reviewed | ||||||
Publication Status: | Published | ||||||
Access rights to Published version: | Restricted or Subscription Access |
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