Effects of Vibrational and Rotational Excitations on Dissociative Chemisorption Dynamics of N2 on Fe(111) |
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Authors: | Huixia Shi Tianhui Liu Yanlin Fu Hao Wu Bina Fu Dong H Zhang |
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Institution: | a.Zhang Dayu School of Chemistry, Dalian University of Technology, Dalian 116024, Chinab.State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China |
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Abstract: | The dissociative chemisorption of N\begin{document}$ _2 $\end{document} is the rate-limiting step for ammonia synthesis in industry. Here, we investigated the role of initially vibrational excitation and rotational excitation of N\begin{document}$ _2 $\end{document} for its reactivity on the Fe(111) surface, based on a recently developed six-dimensional potential energy surface. Six-dimensional quantum dynamics study was carried out to investigate the effect of vibrational excitation for incidence energy below 1.6 eV, due to significant quantum effects for this reaction. The effects of vibrational and rotational excitations at high incidence energies were revealed by quasiclassical trajectory calculations. We found that raising the translational energy can enhance the dissociation probability to some extent, however, the vibrational excitation or rotational excitation can promote dissociation more efficiently than the same amount of translational energy. This study provides valuable insight into the mode-specific dynamics of this heavy diatom-surface reaction. |
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Keywords: | Quantum dynamics Quasiclassical trajectory Dissociative chemisorption Vibrational excitation Rotational excitation |
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