Liu, Xi, Conte, Marco, He, Qian ORCID: https://orcid.org/0000-0003-4891-3581, Knight, David W., Murphy, Damien M. ORCID: https://orcid.org/0000-0002-5941-4879, Taylor, Stuart H. ORCID: https://orcid.org/0000-0002-1933-4874, Whiston, Keith, Kiely, Christopher J. ORCID: https://orcid.org/0000-0001-5412-0970 and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2017. Catalytic partial oxidation of cyclohexane by bimetallic Ag/Pd nanoparticles on magnesium oxide. Chemistry - A European Journal 23 (49) 10.1002/chem.201605941 |
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Abstract
The liquid-phase oxidation of cyclohexane to cyclohexanol and cyclohexanone was investigated by synthesizing and testing an array of heterogeneous catalysts comprising: monometallic Ag/MgO, monometallic Pd/MgO and a set of bimetallic AgPd/MgO catalysts. Interestingly, Ag/MgO was capable of a conversion comparable to current industrial routes of approximately 5 %, and with a high selectivity (up to 60 %) to cyclohexanol, thus making Ag/MgO an attractive system for the synthesis of intermediates for the manufacture of nylon fibres. Furthermore, following the doping of Ag nanoparticles with Pd, the conversion increased up to 10 % whilst simultaneously preserving a high selectivity to the alcohol. Scanning transmission electron microscopy and energy dispersive spectroscopy of the catalysts showed a systematic particle-size-composition variation with the smaller Ag–Pd nanoparticles being statistically richer in Pd. Analysis of the reaction mixture by electron paramagnetic resonance (EPR) spectroscopy coupled with the spin-trapping technique showed the presence of large amounts of alkoxy radicals, thus providing insights for a possible reaction mechanism.
Item Type: | Article |
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Date Type: | Publication |
Status: | Published |
Schools: | Chemistry Cardiff Catalysis Institute (CCI) |
Uncontrolled Keywords: | cyclohexane oxidation; silver palladium catalysts |
Publisher: | Wiley |
ISSN: | 0947-6539 |
Date of First Compliant Deposit: | 16 March 2017 |
Date of Acceptance: | 7 March 2017 |
Last Modified: | 06 Nov 2024 18:16 |
URI: | https://orca.cardiff.ac.uk/id/eprint/99074 |
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