title: Design of Highly Selective Platinum Nanoparticle Catalysts for the Aerobic Oxidation of KA-Oil using Continuous-Flow Chemistry.
abstract: Highly active and selective aerobic oxidation of KA-oil to cyclohexanone (precursor for adipic acid and ɛ-caprolactam) has been achieved in high yields using continuous-flow chemistry by utilizing uncapped noble-metal (Au, Pt & Pd) nanoparticle catalysts. These are prepared using a one-step in situ methodology, within three-dimensional porous molecular architectures, to afford robust heterogeneous catalysts. Detailed spectroscopic characterization of the nature of the active sites at the molecular level, coupled with aberration-corrected scanning transmission electron microscopy, reveals that the synthetic methodology and associated activation procedures play a vital role in regulating the morphology, shape and size of the metal nanoparticles. These active centers have a profound influence on the activation of molecular oxygen for selective catalytic oxidations.
authors.affiliation: University of Southampton, Southampton, SO17 1BJ, UK.
authors.forename: Arran M
authors.initials: AM
authors.lastname: Gill
authors.affiliation: University of Southampton, Southampton, SO17 1BJ, UK.
authors.forename: Christopher S
authors.initials: CS
authors.lastname: Hinde
authors.affiliation: University of Cambridge, Cambridge, CB3 0FS, UK.
authors.forename: Rowan K
authors.initials: RK
authors.lastname: Leary
authors.affiliation: University of Southampton, Southampton, SO17 1BJ, UK.|Georgia Institute of Technology, Atlanta, 30332-0100, USA.
authors.forename: Matthew E
authors.initials: ME
authors.lastname: Potter
authors.affiliation: University of Southampton, Southampton, SO17 1BJ, UK.|University of Turin, Via P. Giuria 7, 10125, Turin, Italy.
authors.forename: Andrea
authors.initials: A
authors.lastname: Jouve
authors.affiliation: UK Catalysis Hub, Oxford, OX11 0FA, UK.|University College London, London, WC1H 0AJ, UK.
authors.forename: Peter P
authors.initials: PP
authors.lastname: Wells
authors.affiliation: University of Cambridge, Cambridge, CB3 0FS, UK.
authors.forename: Paul A
authors.initials: PA
authors.lastname: Midgley
authors.affiliation: University of Cambridge, Cambridge, CB3 0FS, UK.
authors.forename: John M
authors.initials: JM
authors.lastname: Thomas
authors.affiliation: University of Southampton, Southampton, SO17 1BJ, UK. R.Raja@soton.ac.uk.
authors.forename: Robert
authors.initials: R
authors.lastname: Raja
mesh_terms: D000332:Aerobiosis; D003510:Cyclohexanes / Q000737:chemistry; D053768:Metal Nanoparticles / Q000737:chemistry*; D009821:Oils / Q000737:chemistry*; D010084:Oxidation-Reduction; D010984:Platinum / Q000737:chemistry*
chemical_list: D003510:Cyclohexanes; D009821:Oils; C506365:Cyclohexane; D010984:Platinum
keywords: aerobic oxidation; flow chemistry; heterogeneous catalysis; nanoparticles; selectivity