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Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle

Promoters are important in catalysis, but the atomistic details of their function and particularly their role in reaction instabilities such as kinetic phase transitions and oscillations are often unknown. Employing hydrogen oxidation as probe reaction, a Rh nanotip for mimicking a single Rh nanopar...

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Autores principales: Raab, Maximilian, Zeininger, Johannes, Suchorski, Yuri, Genest, Alexander, Weigl, Carla, Rupprechter, Günther
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10632447/
https://www.ncbi.nlm.nih.gov/pubmed/37938552
http://dx.doi.org/10.1038/s41467-023-43026-3
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author Raab, Maximilian
Zeininger, Johannes
Suchorski, Yuri
Genest, Alexander
Weigl, Carla
Rupprechter, Günther
author_facet Raab, Maximilian
Zeininger, Johannes
Suchorski, Yuri
Genest, Alexander
Weigl, Carla
Rupprechter, Günther
author_sort Raab, Maximilian
collection PubMed
description Promoters are important in catalysis, but the atomistic details of their function and particularly their role in reaction instabilities such as kinetic phase transitions and oscillations are often unknown. Employing hydrogen oxidation as probe reaction, a Rh nanotip for mimicking a single Rh nanoparticle and field electron microscopy for in situ monitoring, we demonstrate a La-mediated local catalytic effect. The oscillatory mode of the reaction provides a tool for studying the interplay between different types of reaction pacemakers, i.e., specific local surface atomic configurations that initiate kinetic transitions. The presence of La shifts the bistable reaction states, changes the oscillation pattern and deactivates one of two pacemaker types for the La-free surface. The observed effects originate from the La-enhanced oxygen activation on the catalyst. The experimental observations are corroborated by micro-kinetic model simulations comprising a system of 25 coupled oscillators.
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spelling pubmed-106324472023-11-10 Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle Raab, Maximilian Zeininger, Johannes Suchorski, Yuri Genest, Alexander Weigl, Carla Rupprechter, Günther Nat Commun Article Promoters are important in catalysis, but the atomistic details of their function and particularly their role in reaction instabilities such as kinetic phase transitions and oscillations are often unknown. Employing hydrogen oxidation as probe reaction, a Rh nanotip for mimicking a single Rh nanoparticle and field electron microscopy for in situ monitoring, we demonstrate a La-mediated local catalytic effect. The oscillatory mode of the reaction provides a tool for studying the interplay between different types of reaction pacemakers, i.e., specific local surface atomic configurations that initiate kinetic transitions. The presence of La shifts the bistable reaction states, changes the oscillation pattern and deactivates one of two pacemaker types for the La-free surface. The observed effects originate from the La-enhanced oxygen activation on the catalyst. The experimental observations are corroborated by micro-kinetic model simulations comprising a system of 25 coupled oscillators. Nature Publishing Group UK 2023-11-08 /pmc/articles/PMC10632447/ /pubmed/37938552 http://dx.doi.org/10.1038/s41467-023-43026-3 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Raab, Maximilian
Zeininger, Johannes
Suchorski, Yuri
Genest, Alexander
Weigl, Carla
Rupprechter, Günther
Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title_full Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title_fullStr Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title_full_unstemmed Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title_short Lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
title_sort lanthanum modulated reaction pacemakers on a single catalytic nanoparticle
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10632447/
https://www.ncbi.nlm.nih.gov/pubmed/37938552
http://dx.doi.org/10.1038/s41467-023-43026-3
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