Journal
CHEMICAL SCIENCE
Volume 4, Issue 8, Pages 3249-3254Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3sc51040a
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Funding
- National Science Foundation [CHE-0910828]
- National Science Foundation of China [21221064, 21073229, 21133006, 91021010]
- Chinese Ministry of Science and Technology [2013CB834601]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0910828] Funding Source: National Science Foundation
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Dissociative chemisorption of CH4 on transition-metal surfaces, representing the rate-limiting step in methane steam reforming, has been shown experimentally to be strongly mode selective. To understand the mode selectivity, a twelve-dimensional global potential energy surface is developed for CH4 interacting with a rigid Ni(111) surface based on a large number of density functional theory points. The reaction dynamics is investigated using an eight-dimensional quantum model, which includes representatives of all four vibrational modes of methane. After correcting for surface effects, key experimental observations, including the mode selectivity, are well reproduced. These theoretical results, along with mechanistic analysis, provide insights into this industrially important heterogeneous reaction.
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