Parlett, CMA, Bruce, DW, Hondow, NS et al. (3 more authors) (2013) Mesoporous silicas as versatile supports to tune the palladium-catalyzed selective aerobic oxidation of allylic alcohols. ChemCatChem, 5 (4). 939 - 950. ISSN 1867-3880
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 SiO 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.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Keywords: | Heterogeneous catalysis; mesoporous materials; nanoparticles; palladium; selective oxidation |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemical & Process Engineering (Leeds) > Institute for Materials Research (Leeds) The University of York > Faculty of Sciences (York) > Chemistry (York) |
Depositing User: | Symplectic Publications |
Date Deposited: | 19 May 2014 10:20 |
Last Modified: | 25 Apr 2015 06:39 |
Published Version: | http://dx.doi.org/10.1002/cctc.201200301 |
Status: | Published |
Publisher: | Wiley-VCH-Verlag |
Identification Number: | 10.1002/cctc.201200301 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:78987 |