期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 5, 期 8, 页码 1294-1299出版社
AMER CHEMICAL SOC
DOI: 10.1021/jz500233n
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- Stichting Nationale Computerfaciliteiten (NCF)
- CW-NWO
- Division of Chemical Sciences, Office of Basic Energy Sciences, Office of Energy Research, U.S. Department of Energy [DE-FG02-87ER13744]
- Swiss National Science Foundation [146487/1]
- Ecole Polytechnique Federale de Lausanne
- Grants-in-Aid for Scientific Research [25887002] Funding Source: KAKEN
The dissociative chemisorption of methane on metal surfaces is of fundamental and practical interest, being a rate-limiting step in the steam reforming process. The reaction is best modeled with quantum dynamics calculations, but these are currently not guaranteed to produce accurate results because they rely on potential energy surfaces based on untested density functionals and on untested dynamical approximations. To help overcome these limitations, here we present for the first time statistically accurate reaction probabilities obtained with ab initio molecular dynamics (AIMD) for a polyatomic gas-phase molecule reacting with a metal surface. Using a general purpose density functional, the AIMD reaction probabilities are in semiquantitative agreement with new quantum-state-resolved experiments on CHID3 + Pt(111). The comparison suggests the use of the sudden approximation for treating the rotations even though CHD3 has large rotational constants and yields an estimated reaction barrier of 0.9 eV for CH4 + Pt(111).
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