In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature

Zongyuan Liu, Pablo Lustemberg, Ramón A. Gutiérrez, John J. Carey, Robert M. Palomino, Mykhailo Vorokhta, David C. Grinter, Pedro J. Ramírez, Vladimír Matolín, Michael Nolan, M. Verónica Ganduglia-Pirovano, Sanjaya D. Senanayake, José A. Rodriguez

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51 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)13041-13046
Number of pages6
JournalAngewandte Chemie - International Edition
Volume56
Issue number42
Early online date16 Aug 2017
DOIs
Publication statusPublished - 9 Oct 2017

Keywords

  • ceria
  • cobalt
  • density functional theory
  • methane dissociation
  • XPS

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    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., & 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 - International Edition, 56(42), 13041-13046. https://doi.org/10.1002/anie.201707538