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Title: Atomic and molecular adsorption on Fe(110)

Abstract

Iron is the principal catalyst for the ammonia synthesis process and the Fischer–Tropsch process, as well as many other heterogeneously catalyzed reactions. It is thus of fundamental importance to understand the interactions between the iron surface and various reaction intermediates. Here in this paper, we present a systematic study of atomic and molecular adsorption behavior over Fe(110) using periodic, self-consistent density functional theory (DFT-GGA) calculations. The preferred binding sites, binding energies, and the corresponding surface deformation energies of five atomic species (H, C, N, O, and S), six molecular species (NH 3, CH 4, N 2, CO, HCN, and NO), and eleven molecular fragments (CH, CH 2, CH 3, NH, NH 2, OH, CN, COH, HCO, NOH, and HNO) were determined on the Fe(110) surface at a coverage of 0.25 monolayer. The binding strengths calculated using the PW91 functional decreased in the following order: C> CH > N > O > S > NH > COH > CN > CH2 > NOH > OH > HNO > HCO > NH2 > H > NO > HCN > CH 3 > CO > N 2 > NH 3. No stable binding structures were observed for CH 4. The estimated diffusion barriersmore » and pathways, as well as the adsorbate-surface and intramolecular vibrational modes of all the adsorbates at their preferred binding sites, were identified. Using the calculated adsorption energetics, we constructed the potential energy surfaces for a few surface reactions including the decomposition of methane, ammonia, dinitrogen, carbon monoxide, and nitric oxide. These potential energy surfaces provide valuable insight into the ability of Fe(110) to catalyze common elementary steps.« less

Authors:
 [1];  [1];  [1];  [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
National Energy Research Scientific Computing Center (NERSC); the Center for Nanoscale Materials (CNM) at Argonne National Laboratory (ANL); and the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility at Pacific Northwest National Laboratory (PNNL)
OSTI Identifier:
1398766
Grant/Contract Number:
FG02-05ER15731
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 667; Journal Issue: C; Journal ID: ISSN 0039-6028
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Density functional theory; Iron; Adsorption; Catalysis; Diffusion

Citation Formats

Xu, Lang, Kirvassilis, Demetrios, Bai, Yunhai, and Mavrikakis, Manos. Atomic and molecular adsorption on Fe(110). United States: N. p., 2017. Web. doi:10.1016/j.susc.2017.09.002.
Xu, Lang, Kirvassilis, Demetrios, Bai, Yunhai, & Mavrikakis, Manos. Atomic and molecular adsorption on Fe(110). United States. doi:10.1016/j.susc.2017.09.002.
Xu, Lang, Kirvassilis, Demetrios, Bai, Yunhai, and Mavrikakis, Manos. Tue . "Atomic and molecular adsorption on Fe(110)". United States. doi:10.1016/j.susc.2017.09.002.
@article{osti_1398766,
title = {Atomic and molecular adsorption on Fe(110)},
author = {Xu, Lang and Kirvassilis, Demetrios and Bai, Yunhai and Mavrikakis, Manos},
abstractNote = {Iron is the principal catalyst for the ammonia synthesis process and the Fischer–Tropsch process, as well as many other heterogeneously catalyzed reactions. It is thus of fundamental importance to understand the interactions between the iron surface and various reaction intermediates. Here in this paper, we present a systematic study of atomic and molecular adsorption behavior over Fe(110) using periodic, self-consistent density functional theory (DFT-GGA) calculations. The preferred binding sites, binding energies, and the corresponding surface deformation energies of five atomic species (H, C, N, O, and S), six molecular species (NH3, CH4, N2, CO, HCN, and NO), and eleven molecular fragments (CH, CH2, CH3, NH, NH2, OH, CN, COH, HCO, NOH, and HNO) were determined on the Fe(110) surface at a coverage of 0.25 monolayer. The binding strengths calculated using the PW91 functional decreased in the following order: C> CH > N > O > S > NH > COH > CN > CH2 > NOH > OH > HNO > HCO > NH2 > H > NO > HCN > CH3 > CO > N2 > NH3. No stable binding structures were observed for CH4. The estimated diffusion barriers and pathways, as well as the adsorbate-surface and intramolecular vibrational modes of all the adsorbates at their preferred binding sites, were identified. Using the calculated adsorption energetics, we constructed the potential energy surfaces for a few surface reactions including the decomposition of methane, ammonia, dinitrogen, carbon monoxide, and nitric oxide. These potential energy surfaces provide valuable insight into the ability of Fe(110) to catalyze common elementary steps.},
doi = {10.1016/j.susc.2017.09.002},
journal = {Surface Science},
number = C,
volume = 667,
place = {United States},
year = {Tue Sep 12 00:00:00 EDT 2017},
month = {Tue Sep 12 00:00:00 EDT 2017}
}

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