Raab, M., Zeininger, J., Suchorski, Y., Tokuda, K., & Rupprechter, G. (2023). Emergence of chaos in a compartmentalized catalytic reaction nanosystem. Nature Communications, 14, Article 736. https://doi.org/10.1038/s41467-023-36434-y
E165-01-1 - Forschungsgruppe Modellkatalyse und angewandte Katalyse
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Zeitschrift:
Nature Communications
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ISSN:
2041-1723
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Datum (veröffentlicht):
10-Feb-2023
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Verlag:
NATURE PORTFOLIO
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Peer Reviewed:
Ja
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Keywords:
Field emission microscopy; compartmentalized nanosystems; hydrogen oxidation; chaos
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Abstract:
In compartmentalized systems, chemical reactions may proceed in differing ways even in adjacent compartments. In compartmentalized nanosystems, the reaction behaviour may deviate from that observed on the macro- or mesoscale. In situ studies of processes in such nanosystems meet severe experimental challenges, often leaving the field to theoretical simulations. Here, a rhodium nanocrystal surface ...
In compartmentalized systems, chemical reactions may proceed in differing ways even in adjacent compartments. In compartmentalized nanosystems, the reaction behaviour may deviate from that observed on the macro- or mesoscale. In situ studies of processes in such nanosystems meet severe experimental challenges, often leaving the field to theoretical simulations. Here, a rhodium nanocrystal surface consisting of different nm-sized nanofacets is used as a model of a compartmentalized reaction nanosystem. Using field emission microscopy, different reaction modes are observed, including a transition to spatio-temporal chaos. The transitions between different modes are caused by variations of the hydrogen pressure modifying the strength of diffusive coupling between individual nanofacets. Microkinetic simulations, performed for a network of 52 coupled oscillators, reveal the origins of the different reaction modes. Since diffusive coupling is characteristic for many living and non-living compartmentalized systems, the current findings may be relevant for a wide class of reaction systems.
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Projekttitel:
Räumlich-zeitliche Phänomene an Strukturbibliotheken: P 32772-N (FWF Fonds zur Förderung der wissenschaftlichen Forschung (FWF))
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Forschungsschwerpunkte:
Surfaces and Interfaces: 50% Modeling and Simulation: 25% Structure-Property Relationsship: 25%