Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering; University of Wisconsin-Madison Department of Chemical and Biological Engineering
Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
The adsorption of atomic (H, C, N, O, S) and molecular (OH, CHx, NHx, CO, NO, CN, N2, HNO, NOH, HCN, x = 1–3) species at 1/4 monolayer coverage on an extended Ag(111) surface was studied here using periodic density functional theory. Geometries and energies were calculated self-consistently using the PW91 functional; nonself-consistent energies using the RPBE functional are also provided. We analyze the binding energies, binding geometries, estimated diffusion barriers, harmonic vibrational frequencies, and energetic and geometric deformation parameters of these adsorbates, comparing them to experimental and theoretical results whenever possible. PW91 gives binding energies that match experimental binding energies more closely than RPBE, which consistently predicts weaker binding than PW91. The data were then used to construct and analyze thermochemistry-only potential energy pathways for the hydrocarbon-assisted and hydrogen-assisted selective catalytic reduction (SCR) of nitric oxide (NO). These analyses provide preliminary insights into the possible mechanistic paths of the SCR of NO on Ag(111). Specifically, we show that deep dehydrogenation leading to the formation of atomic intermediates is not favored on Ag(111).
Chen, Benjamin W. J., et al. "Atomic and Molecular Adsorption on Ag(111)." Journal of Physical Chemistry. C, vol. 123, no. 13, Jan. 2018. https://doi.org/10.1021/acs.jpcc.7b11629
Chen, Benjamin W. J., Kirvassilis, Demetrios, Bai, Yunhai, & Mavrikakis, Manos (2018). Atomic and Molecular Adsorption on Ag(111). Journal of Physical Chemistry. C, 123(13). https://doi.org/10.1021/acs.jpcc.7b11629
Chen, Benjamin W. J., Kirvassilis, Demetrios, Bai, Yunhai, et al., "Atomic and Molecular Adsorption on Ag(111)," Journal of Physical Chemistry. C 123, no. 13 (2018), https://doi.org/10.1021/acs.jpcc.7b11629
@article{osti_1494745,
author = {Chen, Benjamin W. J. and Kirvassilis, Demetrios and Bai, Yunhai and Mavrikakis, Manos},
title = {Atomic and Molecular Adsorption on Ag(111)},
annote = {The adsorption of atomic (H, C, N, O, S) and molecular (OH, CHx, NHx, CO, NO, CN, N2, HNO, NOH, HCN, x = 1–3) species at 1/4 monolayer coverage on an extended Ag(111) surface was studied here using periodic density functional theory. Geometries and energies were calculated self-consistently using the PW91 functional; nonself-consistent energies using the RPBE functional are also provided. We analyze the binding energies, binding geometries, estimated diffusion barriers, harmonic vibrational frequencies, and energetic and geometric deformation parameters of these adsorbates, comparing them to experimental and theoretical results whenever possible. PW91 gives binding energies that match experimental binding energies more closely than RPBE, which consistently predicts weaker binding than PW91. The data were then used to construct and analyze thermochemistry-only potential energy pathways for the hydrocarbon-assisted and hydrogen-assisted selective catalytic reduction (SCR) of nitric oxide (NO). These analyses provide preliminary insights into the possible mechanistic paths of the SCR of NO on Ag(111). Specifically, we show that deep dehydrogenation leading to the formation of atomic intermediates is not favored on Ag(111).},
doi = {10.1021/acs.jpcc.7b11629},
url = {https://www.osti.gov/biblio/1494745},
journal = {Journal of Physical Chemistry. C},
issn = {ISSN 1932-7447},
number = {13},
volume = {123},
place = {United States},
publisher = {American Chemical Society},
year = {2018},
month = {01}}
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; FG02-05ER15731
OSTI ID:
1494745
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 13 Vol. 123; ISSN 1932-7447
