On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.
The research described in this product was performed in part in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The thermochemical stability of various three-component phases containing oxygen, ethylene, and Ag(111) was determined as a function of oxygen and ethylene chemical potential using periodic, self-consistent density functional theory calculations. Ethylenedioxy is stable over a wide range of conditions, although its formation may be kinetically hindered in some cases. Ethylene and ethylene-containing oxametallacycles are also found to be stable over a reasonably large range of chemical potentials, particularly if ethylenedioxy formation is neglected. Furthermore, subsurface oxygen (Osb) is seen to be present in the three-component systems at a variety of conditions; minimum energy path calculations performed at a coverage of 1/2 ML Osb suggest that this species may actually increase the reaction barrier for ring closure leading to ethylene oxide elimination from Ag(111).
- Research Organization:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 989062
- Journal Information:
- Journal of Physical Chemistry C, 111(22):7992-7999, Journal Name: Journal of Physical Chemistry C, 111(22):7992-7999 Journal Issue: 22 Vol. 111; ISSN 1932-7447
- Country of Publication:
- United States
- Language:
- English
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