Jump to main content
Jump to site search

Issue 10, 2012
Previous Article Next Article

Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations

Author affiliations

Abstract

Room temperature activation of methane over a Zn modified H-ZSM-5 zeolite catalyst was investigated by solid-state NMR spectroscopy in combination with other spectroscopic methods and DFT theoretical calculations. We found for the first time that the activation of methane resulted in the preferential formation of surface methoxy intermediates at room temperature, which mediated the formation of methanol and its further conversion to hydrocarbons. Experimental and theoretical calculation results demonstrated that an oxygen-containing dizinc cluster center in an open shell was responsible for homolytic cleavage of the C–H bond of methane at room temperature, leading to the formation of methyl radicals. The zeolite matrix readily trapped the methyl radicals by forming the surface methoxy intermediates for further selective conversion. In parallel to the homolytic cleavage pathway, heterolytic dissociation of methane was also observed on isolated Zn2+ ions at room temperature, which gives rise to zinc methyl species.

Graphical abstract: Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations

Back to tab navigation

Supplementary files

Publication details

The article was received on 09 Apr 2012, accepted on 01 Jun 2012 and first published on 13 Jun 2012


Article type: Edge Article
DOI: 10.1039/C2SC20434G
Chem. Sci., 2012,3, 2932-2940

  •   Request permissions

    Room temperature activation of methane over Zn modified H-ZSM-5 zeolites: Insight from solid-state NMR and theoretical calculations

    J. Xu, A. Zheng, X. Wang, G. Qi, J. Su, J. Du, Z. Gan, J. Wu, W. Wang and F. Deng, Chem. Sci., 2012, 3, 2932
    DOI: 10.1039/C2SC20434G

Search articles by author

Spotlight

Advertisements