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

• Main Authors: Yeo, Sang Chul (Author), Lo, Yu-Chieh (Author), Li, Ju (Contributor), Lee, Hyuck Mo (Author)
• Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering (Contributor), Massachusetts Institute of Technology. Department of Nuclear Science and Engineering (Contributor), Lo, Yu Chieh (Contributor)
• Format: Article
• Language: English
• Published: American Institute of Physics (AIP), 2015-03-05T19:21:15Z.
• Subjects: Article
• Online Access: Get fulltext

 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.