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Title: On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.

Abstract

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).

Authors:
;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
989062
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physical Chemistry C, 111(22):7992-7999; Journal Volume: 111; Journal Issue: 22
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CLOSURES; ETHYLENE; FUNCTIONALS; OXIDES; OXYGEN; SILVER; STABILITY; Environmental Molecular Sciences Laboratory

Citation Formats

Greeley, Jeffrey P., and Mavrikakis, Manos. On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.. United States: N. p., 2007. Web. doi:10.1021/jp070490i.
Greeley, Jeffrey P., & Mavrikakis, Manos. On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.. United States. doi:10.1021/jp070490i.
Greeley, Jeffrey P., and Mavrikakis, Manos. Sat . "On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.". United States. doi:10.1021/jp070490i.
@article{osti_989062,
title = {On the Role of Subsurface Oxygen and Ethylenedioxy in Ethylene Epoxidation on Silver.},
author = {Greeley, Jeffrey P. and Mavrikakis, Manos},
abstractNote = {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).},
doi = {10.1021/jp070490i},
journal = {Journal of Physical Chemistry C, 111(22):7992-7999},
number = 22,
volume = 111,
place = {United States},
year = {Sat May 12 00:00:00 EDT 2007},
month = {Sat May 12 00:00:00 EDT 2007}
}