Cu-Exchanged Ferrierite Zeolite for the Direct CH4 to CH3OH Conversion: Insights on Cu Speciation from X-Ray Absorption Spectroscopy View Full Text


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

2019-03-15

AUTHORS

Dimitrios K. Pappas, Elisa Borfecchia, Kirill A. Lomachenko, Andrea Lazzarini, Emil S. Gutterød, Michael Dyballa, Andrea Martini, Gloria Berlier, Silvia Bordiga, Carlo Lamberti, Bjørnar Arstad, Unni Olsbye, Pablo Beato, Stian Svelle

ABSTRACT

The direct stepwise transformation of CH4 to CH3OH over Cu-exchanged zeolites has been an intensively researched reaction as it can provide a solution for the utilization of this abundant feedstock. Up to date a commercial process is far from realization, which is why an understanding of the Cu speciation in zeolites as a function of reaction conditions as well as the development of a mechanistic view of the reaction are necessary to further advance the field. Herein we study Cu-exchanged ferrierite zeolite for the direct CH4 to CH3OH conversion by utilizing X-ray absorption spectroscopy (XAS), in order to assess the local structure and electronic properties of Cu through the reaction. A Cu-FER sample with a Cu/Al = 0.20 and Si/Al = 11 was subjected to three reaction cycles yielding ultimately 96 µmolCH3OH/gzeolite. Normalized to the Cu loading, this accounts for 0.33 molCH3OH/molCu, making the sample comparable to very active Cu-MOR materials reported in the literature. During O2 activation, a transient self-reduction regime of CuII to CuI ions was identified; eventually leading to mostly framework interacting CuII species. CH4 loading leads to a reduction of these CuII containing species; which are finally partially reoxidized during H2O-assisted CH3OH extraction. The speciation after CH4 activation as well as H2O-assisted CH3OH extraction was assessed via linear combination fitting analysis of the XAS data. More... »

PAGES

1-12

Identifiers

URI

http://scigraph.springernature.com/pub.10.1007/s11244-019-01160-7

DOI

http://dx.doi.org/10.1007/s11244-019-01160-7

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1112780067


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