Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study
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Author(s)
Yeo, Sang Chul
Lo, Yu-Chieh
Li, Ju
Lee, Hyuck Mo
Date Issued
October 2014
Journal
Journal of Chemical Physics
Publisher
American Institute of Physics (AIP)
Citation
Yeo, Sang Chul, Yu Chieh Lo, Ju Li, and Hyuck Mo Lee. “Theoretical Study of the Ammonia Nitridation Rate on an Fe (100) Surface: A Combined Density Functional Theory and Kinetic Monte Carlo Study.” The Journal of Chemical Physics 141, no. 13 (October 7, 2014): 134108. © 2014 AIP Publishing LLC
Version
Final published version
Abstract
Ammonia (NH[subscript 3]) nitridation on an Fe surface was studied by combining density functional theory (DFT) and kinetic Monte Carlo (kMC) calculations. A DFT calculation was performed to obtain the energy barriers (E[subscript b]) of the relevant elementary processes. The full mechanism of the exact reaction path was divided into five steps (adsorption, dissociation, surface migration, penetration, and diffusion) on an Fe (100) surface pre-covered with nitrogen. The energy barrier (E[subscript b]) depended on the N surface coverage. The DFT results were subsequently employed as a database for the kMC simulations. We then evaluated the NH[subscript 3] nitridation rate on the N pre-covered Fe surface. To determine the conditions necessary for a rapid NH[subscript 3] nitridation rate, the eight reaction events were considered in the kMC simulations: adsorption, desorption, dissociation, reverse dissociation, surface migration, penetration, reverse penetration, and diffusion. This study provides a real-time-scale simulation of NH[subscript 3] nitridation influenced by nitrogen surface coverage that allowed us to theoretically determine a nitrogen coverage (0.56 ML) suitable for rapid NH[subscript 3] nitridation. In this way, we were able to reveal the coverage dependence of the nitridation reaction using the combined DFT and kMC simulations.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Nuclear Science and Engineering
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DOI of Published Version
https://doi.org/10.1063/1.4896610
