Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study

Yeo, Sang Chul; Lo, Yu Chieh; Li, Ju

doi:10.1063/1.4896610

Title: 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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Abstract

Ammonia (NH{sub 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{sub 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{sub 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{sub 3} nitridation rate on the N pre-covered Fe surface. To determine the conditions necessary for a rapid NH{sub 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{sub 3} nitridation influenced by nitrogen surface coverage that allowed us to theoretically determine a nitrogen coverage (0.56 ML) suitable for rapid NH{sub 3} nitridation. In this way, we were able to reveal the coverage dependence of the nitridation reaction using the combined DFT and kMC simulations.

Authors:

Yeo, Sang Chul; Lo, Yu Chieh; Li, Ju ^[1]

Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)

Publication Date:: Tue Oct 07 00:00:00 EDT 2014

OSTI Identifier:: 22436538

Resource Type:: Journal Article

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 141; Journal Issue: 13; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ADSORPTION; AMMONIA; DENSITY FUNCTIONAL METHOD; DESORPTION; DISSOCIATION; MONTE CARLO METHOD; NITRIDATION; SIMULATION

Citation Formats


                    Yeo, Sang Chul, Lee, Hyuck Mo, E-mail: hmlee@kaist.ac.kr, Lo, Yu Chieh, and Li, Ju. Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study.  United States: N. p., 2014. 
        Web.  doi:10.1063/1.4896610.

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                    Yeo, Sang Chul, Lee, Hyuck Mo, E-mail: hmlee@kaist.ac.kr, Lo, Yu Chieh, & Li, Ju. Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study.  United States.  https://doi.org/10.1063/1.4896610

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                    Yeo, Sang Chul, Lee, Hyuck Mo, E-mail: hmlee@kaist.ac.kr, Lo, Yu Chieh, and Li, Ju. 2014.  
        "Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study".  United States.  https://doi.org/10.1063/1.4896610.

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@article{osti_22436538,

  title        = {Theoretical study of the ammonia nitridation rate on an Fe (100) surface: A combined density functional theory and kinetic Monte Carlo study},

  author       = {Yeo, Sang Chul and Lee, Hyuck Mo, E-mail: hmlee@kaist.ac.kr and Lo, Yu Chieh and Li, Ju},

  abstractNote = {Ammonia (NH{sub 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{sub 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{sub 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{sub 3} nitridation rate on the N pre-covered Fe surface. To determine the conditions necessary for a rapid NH{sub 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{sub 3} nitridation influenced by nitrogen surface coverage that allowed us to theoretically determine a nitrogen coverage (0.56 ML) suitable for rapid NH{sub 3} nitridation. In this way, we were able to reveal the coverage dependence of the nitridation reaction using the combined DFT and kMC simulations.},

  doi          = {10.1063/1.4896610},

  url          = {https://www.osti.gov/biblio/22436538},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  number       = 13,

  volume       = 141,

  place        = {United States},

  year         = {Tue Oct 07 00:00:00 EDT 2014},

  month        = {Tue Oct 07 00:00:00 EDT 2014}

}

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