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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
Journal Title
Journal ISSN
Volume Title
Publisher
John Wiley & Sons, Inc.
Published Version
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
Copyright
© 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.