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Pappas DK, Martini A, Dyballa M, et al. The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment. J Am Chem Soc. 2018;140(45):15270-15278doi: 10.1021/jacs.8b08071.
Pappas, D. K., Martini, A., Dyballa, M., Kvande, K., Teketel, S., Lomachenko, K. A., Baran, R., Glatzel, P., Arstad, B., Berlier, G., Lamberti, C., Bordiga, S., Olsbye, U., Svelle, S., Beato, P., & Borfecchia, E. (2018). The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment. Journal of the American Chemical Society, 140(45), 15270-15278. https://doi.org/10.1021/jacs.8b08071
Pappas, Dimitrios K, et al. "The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment." Journal of the American Chemical Society vol. 140,45 (2018): 15270-15278. doi: https://doi.org/10.1021/jacs.8b08071
Pappas DK, Martini A, Dyballa M, Kvande K, Teketel S, Lomachenko KA, Baran R, Glatzel P, Arstad B, Berlier G, Lamberti C, Bordiga S, Olsbye U, Svelle S, Beato P, Borfecchia E. The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment. J Am Chem Soc. 2018 Nov 14;140(45):15270-15278. doi: 10.1021/jacs.8b08071. Epub 2018 Nov 02. PMID: 30346154.
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J Am Chem Soc. 2018 Nov 14;140(45):15270-15278. doi: 10.1021/jacs.8b08071. Epub 2018 Nov 02.

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

Journal of the American Chemical Society

Dimitrios K Pappas, Andrea Martini, Michael Dyballa, Karoline Kvande, Shewangizaw Teketel, Kirill A Lomachenko, Rafal Baran, Pieter Glatzel, Bjørnar Arstad, Gloria Berlier, Carlo Lamberti, Silvia Bordiga, Unni Olsbye, Stian Svelle, Pablo Beato, Elisa Borfecchia

Affiliations

  1. Center for Materials Science and Nanotechnology, Department of Chemistry , University of Oslo , 1033 Blindern , 0315 Oslo , Norway.
  2. IRC "Smart Materials" , Southern Federal University , Zorge Street 5 , 344090 Rostov-on-Don , Russia.
  3. SINTEF Industry , Forskningsveien 1 , 0373 Oslo , Norway.
  4. Haldor Topsøe A/S , Haldor Topsøes Allé 1 , 2800 Kongens Lyngby , Denmark.
  5. European Synchrotron Radiation Facility , 71 avenue des Martyrs , CS 40220, 38043 Grenoble Cedex 9 , France.

PMID: 30346154 DOI: 10.1021/jacs.8b08071

Abstract

The direct conversion of methane to methanol (MTM) is a reaction that has the potential to disrupt a 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 data to accurately quantify the fraction of active Cu in Cu-MOR (MOR = mordenite), allowing an unambiguous determination of the active site nuclearity as a dicopper 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.

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