期刊
CHEMPHYSCHEM
卷 21, 期 7, 页码 673-679出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201900973
关键词
C-H activation; methane; methanol; zeolites; zinc
资金
- EPSRC [EP/R01213X/1]
- Durham University
- EPSRC [EP/R01213X/1] Funding Source: UKRI
The first selective oxidation of methane to methanol is reported herein for zinc-exchanged MOR (Zn/MOR). Under identical conditions, Zn/FER and Zn/ZSM-5 both form zinc formate and methanol. Selective methane activation to form [Zn-CH3](+) species was confirmed by C-13 MAS NMR spectroscopy for all three frameworks. The percentage of active zinc sites, measured through quantitative NMR spectroscopy studies, varied with the zeolite framework and was found to be ZSM-5 (5.7 %), MOR (1.2 %) and FER (0.5 %). For Zn/MOR, two signals were observed in the C-13 MAS NMR spectrum, resulting from two distinct [Zn-CH3](+) species present in the 12 MR and 8 MR side pockets, as supported by additional NMR experiments. The observed products of oxidation of the [Zn-CH3](+) species are shown to depend on the zeolite framework type and the oxidative conditions used. These results lay the foundation for developing structure-function correlations for methane conversion over zinc-exchanged zeolites.
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