期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 23, 期 49, 页码 11834-11842出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201605941
关键词
cyclohexane oxidation; EPR spectroscopy; palladium; silver; scanning transmission electron microscopy (STEM)
资金
- INVISTA Textiles (UK) Limited
- National Science Foundation Major Research Instrumentation Programme [MRI/DMR-1040229]
- National Nature Science Foundation of China [21673273]
- EPSRC [EP/K017322/1] Funding Source: UKRI
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.
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