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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
Author(s) -
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,
GandugliaPirovano M. Verónica,
Senanayake Sanjaya D.,
Rodriguez José A.
Publication year - 2017
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201707538
Subject(s) - methane , catalysis , oxide , metal , carbon dioxide reforming , x ray photoelectron spectroscopy , chemistry , inorganic chemistry , materials science , chemical engineering , syngas , organic chemistry , engineering
Studies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO 2 ) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO 2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO 2 (111) exhibits the best performance and Cu/CeO 2 (111) has negligible activity. Experiments using ambient pressure X‐ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO 2 (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 Co 2+ /CeO 2 (111), and to only 0.05 eV on Co 0 /CeO 2− x (111). At 700 K, under methane dry reforming conditions, CO 2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CH x formed on the Co 0 /CeO 2− x (111) catalyst recombines to yield ethane or ethylene.