In situ investigation of methane dry reforming on metal/ceria(111) surfaces: metal-support interactions and C-H bond activation at low temperature
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Accepted Version
Date
2017-09-05
Authors
Liu, Zongyuan
Lustemberg, Pablo
Gutiérrez, Ramón A.
Carey, John J.
Palomino, Robert M.
Vorokhta, Mykhailo
Grinter, David C.
Ramírez, Pedro J.
Matolín, Vladimír
Nolan, Michael
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Volume Title
Publisher
John Wiley & Sons, Inc.
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Abstract
Studies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO2) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO2(111) exhibits the best performance and Cu/CeO2(111) has negligible activity. Experiments using ambient pressure X-ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO2(111) at temperatures as low as 300 K—generating CHx and COx species on the catalyst surface. The results of density functional calculations show a reduction in the methane activation barrier from 1.07 eV on Co(0001) to 0.87 eV on Co2+/CeO2(111), and to only 0.05 eV on Co0/CeO2−x(111). At 700 K, under methane dry reforming conditions, CO2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CHx formed on the Co0/CeO2−x(111) catalyst recombines to yield ethane or ethylene.
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Keywords
Cobalt , XPS , Density functional theory , Methane dissociation , Ceria
Citation
Liu, Z., Lustemberg, P., Gutiérrez, R. A., Carey, J. J., Palomino, R. M., Vorokhta, M., Grinter, D. C., Ramírez, P. J., Matolín, V., Nolan, M., Ganduglia-Pirovano, M. V., Senanayake, S. D. and Rodriguez, J. A. (2017) ‘In situ investigation of methane dry reforming on metal/ceria(111) surfaces: metal-support interactions and C-H bond activation at low temperature’, Angewandte Chemie, 129(42), pp. 13221-13226. doi:10.1002/ange.201707538
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© 2017, John Wiley & Sons Ltd. This peer reviewed manuscript has been published in final form at http://dx.doi.org/10.1002/ange.201707538. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.