The direct conversion of methane to methanol (MTM) is a reaction which has the potential to disrupt great part of the synthesis gas derived chemical industry. However, despite many decades of research, active enough catalysts and suitable processes for industrial application are still not available. Recently, several copper-exchanged zeolites have shown considerable activity and selectivity in the direct MTM reaction. Understanding the nature of the active site in these materials is essential for any further development in the field. Herein, we apply multivariate curve resolution analysis of X-ray absorption spectroscopy (XAS) data to accurately quantify the fraction of active Cu in Cu-MOR, allowing an unambiguous determination of the active site nuclearity as a di-copper site. By rationalizing the compositional parameters and reaction conditions, we achieve the highest methanol yield per Cu yet reported for MTM over Cu-zeolites, of 0.47 mol/mol.

The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment

Martini, Andrea;Berlier, Gloria;Lamberti, Carlo;Bordiga, Silvia;Borfecchia, Elisa
2018-01-01

Abstract

The direct conversion of methane to methanol (MTM) is a reaction which has the potential to disrupt great part of the synthesis gas derived chemical industry. However, despite many decades of research, active enough catalysts and suitable processes for industrial application are still not available. Recently, several copper-exchanged zeolites have shown considerable activity and selectivity in the direct MTM reaction. Understanding the nature of the active site in these materials is essential for any further development in the field. Herein, we apply multivariate curve resolution analysis of X-ray absorption spectroscopy (XAS) data to accurately quantify the fraction of active Cu in Cu-MOR, allowing an unambiguous determination of the active site nuclearity as a di-copper site. By rationalizing the compositional parameters and reaction conditions, we achieve the highest methanol yield per Cu yet reported for MTM over Cu-zeolites, of 0.47 mol/mol.
2018
140
45
15270
15278
http://pubs.acs.org/journal/jacsat
Catalysis; Cu-zeolites, methane to methanol conversion, synchrotron, XAS, HERFD-XANES, MCR
Pappas, Dimitrios K.; Martini, Andrea; Dyballa, Michael; Kvande, Karoline; Teketel, Shewangizaw; Lomachenko, Kirill A.; Baran, Rafal; Glatzel, Pieter;...espandi
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/1692616
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