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- Title
In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal-Support Interactions and C−H Bond Activation at Low Temperature.
- 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; Ganduglia‐Pirovano, M. Verónica; Senanayake, Sanjaya D.; Rodriguez, José A.
- 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 CH x and CO x 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 CH x formed on the Co0/CeO2− x(111) catalyst recombines to yield ethane or ethylene.
- Subjects
METHANE; HYDROGEN bonding; METALLIC oxides; CERIUM oxides; X-ray photoelectron spectroscopy
- Publication
Angewandte Chemie, 2017, Vol 129, Issue 42, p13221
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201707538