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The selective oxidation of cyclohexane via in-situ H2O2 production over supported Pd-based catalysts

DOI: 10.1007/s10562-020-03511-6 DOI Help

Authors: Caitlin M. Crombie (Cardiff University) , Richard J. Lewis (Cardiff University) , Dávid Kovačič (Cardiff University) , David J. Morgan (Cardiff University; HarwellXPS, Research Complex At Harwell (RCaH)) , Thomas J. A. Slater (Diamond Light Source) , Thomas E. Davies (Cardiff University) , Jennifer. K. Edwards (Cardiff University) , Martin Skov Skjøth-Rasmussen (Haldor Topsøe A/S) , Graham J. Hutchings (Cardiff University)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Catalysis Letters , VOL 12

State: Published (Approved)
Published: January 2021
Diamond Proposal Number(s): 26190

Open Access Open Access

Abstract: The oxidation of cyclohexane via the in-situ production of H2O2 from molecular H2 and O2 offers an attractive route to the current industrial means of producing cyclohexanone and cyclohexanol (KA oil), key materials in the production of Nylon. The in-situ route has the potential to overcome the significant economic and environmental concerns associated with the use of commercial H2O2, while also allowing for the use of far lower reaction temperatures than those typical of the purely aerobic route to KA oil. Herein we demonstrate the efficacy of a series of bi-functional Pd-based catalysts, which offer appreciable concentrations of KA oil, under conditions where limited activity is observed using O2 alone. In particular the introduction of V into a supported Pd catalyst is seen to improve KA oil concentration by an order of magnitude, compared to the Pd-only analogue. In particular we ascribe this improvement in catalytic performance to the development of Pd domains of mixed oxidation state upon V incorporation as evidenced through X-ray photoelectron spectroscopy.

Journal Keywords: Palladium; Vanadium; Hydrogen peroxide; Cyclohexane oxidation; Green chemistry

Subject Areas: Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E01-JEM ARM 200CF

Added On: 25/01/2021 14:40

Documents:
Crombie2021_Article_TheSelectiveOxidationOfCyclohe.pdf

Discipline Tags:

Catalysis Organic Chemistry Physical Chemistry Chemistry

Technical Tags:

Microscopy Electron Microscopy (EM) Scanning Transmission Electron Microscopy (STEM)