Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles
Abstract 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)...
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56765-2 |
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| author | Yuqi Yang Anders Hellman Henrik Grönbeck |
| author_facet | Yuqi Yang Anders Hellman Henrik Grönbeck |
| author_sort | Yuqi Yang |
| collection | DOAJ |
| description | Abstract 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. |
| format | Article |
| id | doaj-art-b007a4a1ad1142f99c5c596c66529ccd |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-b007a4a1ad1142f99c5c596c66529ccd2025-08-20T02:48:12ZengNature PortfolioNature Communications2041-17232025-02-011611810.1038/s41467-025-56765-2Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticlesYuqi Yang0Anders Hellman1Henrik Grönbeck2Department of Physics and Competence Centre for Catalysis, Chalmers University of TechnologyDepartment of Physics and Competence Centre for Catalysis, Chalmers University of TechnologyDepartment of Physics and Competence Centre for Catalysis, Chalmers University of TechnologyAbstract 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.https://doi.org/10.1038/s41467-025-56765-2 |
| spellingShingle | Yuqi Yang Anders Hellman Henrik Grönbeck Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles Nature Communications |
| title | Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles |
| title_full | Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles |
| title_fullStr | Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles |
| title_full_unstemmed | Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles |
| title_short | Inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over Ru nanoparticles |
| title_sort | inherent strain and kinetic coupling determine the kinetics of ammonia synthesis over ru nanoparticles |
| url | https://doi.org/10.1038/s41467-025-56765-2 |
| work_keys_str_mv | AT yuqiyang inherentstrainandkineticcouplingdeterminethekineticsofammoniasynthesisoverrunanoparticles AT andershellman inherentstrainandkineticcouplingdeterminethekineticsofammoniasynthesisoverrunanoparticles AT henrikgronbeck inherentstrainandkineticcouplingdeterminethekineticsofammoniasynthesisoverrunanoparticles |