Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles
Journal article, 2025

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.

Author

Yuqi Yang

Chalmers, Physics, Chemical Physics

Anders Hellman

Chalmers, Physics, Chemical Physics

Henrik Grönbeck

Chalmers, Physics, Chemical Physics

Nature Communications

2041-1723 (ISSN) 20411723 (eISSN)

Vol. 16 1 1625

Adaptive multiscale modeling in heterogeneous catalysis

Swedish Research Council (VR) (2020-05191), 2021-01-01 -- 2024-12-31.

Areas of Advance

Nanoscience and Nanotechnology

Subject Categories (SSIF 2025)

Condensed Matter Physics

Organic Chemistry

DOI

10.1038/s41467-025-56765-2

PubMed

39948080

Related datasets

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

URI: https://doi.org/10.5281/zenodo.14670930

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3/7/2025 9