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<p>The large-scale ammonia synthesis using the Haber-Bosch process is crucial in modern society and the reaction is known to be facile over Ru-based catalysts. Herein, first-principles kinetic Monte Carlo (kMC) simulations are utilized to explore the reaction kinetics on Ru nanoparticles (NPs), extending the current knowledge that is mainly based on calculations of single crystal surfaces. It is only by accounting for the effects of kinetic couplings between different sites and inherent strain in the NPs that experimental turnover frequencies (TOFs) can be reproduced. The enhanced activity of inherently strained NPs is attributed to the co-existence of sites with both tensile and compressive strain, which simultaneously promotes N<sub>2</sub> dissociation and NH<sub>x</sub> (x = 0, 1 and 2) hydrogenation. We propose that kinetic couplings on Ru NPs with tailored strain-patterns offer a strategy to break the limitations of linear scaling relations in the design of ammonia synthesis catalysts.</p>

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Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年2月13日

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  • Yuqi Yang,
  • Anders Hellman,
  • Henrik Grönbeck

摘要

The large-scale ammonia synthesis using the Haber-Bosch process is crucial in modern society and the reaction is known to be facile over Ru-based catalysts. Herein, first-principles kinetic Monte Carlo (kMC) simulations are utilized to explore the reaction kinetics on Ru nanoparticles (NPs), extending the current knowledge that is mainly based on calculations of single crystal surfaces. It is only by accounting for the effects of kinetic couplings between different sites and inherent strain in the NPs that experimental turnover frequencies (TOFs) can be reproduced. The enhanced activity of inherently strained NPs is attributed to the co-existence of sites with both tensile and compressive strain, which simultaneously promotes N2 dissociation and NHx (x = 0, 1 and 2) hydrogenation. We propose that kinetic couplings on Ru NPs with tailored strain-patterns offer a strategy to break the limitations of linear scaling relations in the design of ammonia synthesis catalysts.