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 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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