Mesoporous silicas as versatile supports to tune the palladium-catalyzed selective aerobic oxidation of allylic alcohols

Christopher M.A. Parlett, Duncan W. Bruce, Nicole S. Hondow, Mark A. Newton, Adam F. Lee, Karen Wilson

Research output: Contribution to journalArticle

Abstract

Surfactant templating offers a simple route to synthesize high-surface area silicas with ordered, tunable mesopore architectures. The use of these materials as versatile catalyst supports for palladium nanoparticles has been explored in the aerobic selective oxidation (selox) of allylic alcohols under mild conditions. Families of Pd/mesoporous silicas, synthesized through incipient wetness impregnation of SBA-15, SBA-16, and KIT-6, have been characterized by using nitrogen porosimetry, CO chemisorption, diffuse reflection infrared Fourier transform spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and high-resolution TEM and benchmarked in liquid phase allylic alcohol selox against a Pd/amorphous SiO2 standard. The transition from amorphous to two-dimensional parallel and three-dimensional interpenetrating porous silica networks conferred significant selox rate enhancements associated with higher surface densities of active palladium oxide sites. Dissolved oxygen was essential for insitu stabilization of palladium oxide, and thus maintenance of high activity on-stream, whereas selectivity to the desired aldehyde selox product over competing hydrogenolysis pathways was directed by using palladium metal.

Original languageEnglish
Pages (from-to)939-950
Number of pages12
JournalChemCatChem
Volume5
Issue number4
Early online date17 Sep 2012
DOIs
Publication statusPublished - Apr 2013

Keywords

  • heterogeneous catalysis
  • mesoporous materials
  • nanoparticles
  • palladium
  • selective oxidation

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