Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction

We studied the catalytic NO2(g) + H2(g)/Pt system on model platinum catalysts with nanoscale spatial resolution by means of field emission microscopy (FEM). While the surface of the catalyst is in a non-reactive state at low H2 partial pressure, bursts of activity are observed when increasing this p...

Cur síos iomlán

Sonraí bibleagrafaíochta
Príomhchruthaitheoirí: Barroo, C, Voorsluijs, V, Visart De Bocarmé, T, Gaspard, P, De Decker, Y
Formáid: Journal article
Teanga:English
Foilsithe / Cruthaithe: Royal Society of Chemistry 2018
_version_ 1826269925156585472
author Barroo, C
Voorsluijs, V
Visart De Bocarmé, T
Gaspard, P
De Decker, Y
author_facet Barroo, C
Voorsluijs, V
Visart De Bocarmé, T
Gaspard, P
De Decker, Y
author_sort Barroo, C
collection OXFORD
description We studied the catalytic NO2(g) + H2(g)/Pt system on model platinum catalysts with nanoscale spatial resolution by means of field emission microscopy (FEM). While the surface of the catalyst is in a non-reactive state at low H2 partial pressure, bursts of activity are observed when increasing this parameter. These kinetic instabilities subsequently evolve towards self-sustained periodic oscillations for a wide range of pressures. Combining time series analyses and numerical simulations of a simple reaction model, we clarify how these observations fit in the traditional classification of dynamical systems. In particular, reconstructions of the probability density around oscillating trajectories show that the experimental system defines a crater-like structure in probability space. The experimental observations thus correspond to a noise-perturbed limit cycle emerging from a nanometric reactive system. This conclusion is further supported by comparison with stochastic simulations of the proposed chemical model. The obtained results and simulations pave the way towards a better understanding of reactive nanosystems.
first_indexed 2024-03-06T21:32:49Z
format Journal article
id oxford-uuid:453f212b-f7d0-472a-a44a-3ab363dce773
institution University of Oxford
language English
last_indexed 2024-03-06T21:32:49Z
publishDate 2018
publisher Royal Society of Chemistry
record_format dspace
spelling oxford-uuid:453f212b-f7d0-472a-a44a-3ab363dce7732022-03-26T15:06:39ZReconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reactionJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:453f212b-f7d0-472a-a44a-3ab363dce773EnglishSymplectic Elements at OxfordRoyal Society of Chemistry2018Barroo, CVoorsluijs, VVisart De Bocarmé, TGaspard, PDe Decker, YWe studied the catalytic NO2(g) + H2(g)/Pt system on model platinum catalysts with nanoscale spatial resolution by means of field emission microscopy (FEM). While the surface of the catalyst is in a non-reactive state at low H2 partial pressure, bursts of activity are observed when increasing this parameter. These kinetic instabilities subsequently evolve towards self-sustained periodic oscillations for a wide range of pressures. Combining time series analyses and numerical simulations of a simple reaction model, we clarify how these observations fit in the traditional classification of dynamical systems. In particular, reconstructions of the probability density around oscillating trajectories show that the experimental system defines a crater-like structure in probability space. The experimental observations thus correspond to a noise-perturbed limit cycle emerging from a nanometric reactive system. This conclusion is further supported by comparison with stochastic simulations of the proposed chemical model. The obtained results and simulations pave the way towards a better understanding of reactive nanosystems.
spellingShingle Barroo, C
Voorsluijs, V
Visart De Bocarmé, T
Gaspard, P
De Decker, Y
Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title_full Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title_fullStr Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title_full_unstemmed Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title_short Reconstructing stochastic attractors from nanoscale experiments on a non-equilibrium reaction
title_sort reconstructing stochastic attractors from nanoscale experiments on a non equilibrium reaction
work_keys_str_mv AT barrooc reconstructingstochasticattractorsfromnanoscaleexperimentsonanonequilibriumreaction
AT voorsluijsv reconstructingstochasticattractorsfromnanoscaleexperimentsonanonequilibriumreaction
AT visartdebocarmet reconstructingstochasticattractorsfromnanoscaleexperimentsonanonequilibriumreaction
AT gaspardp reconstructingstochasticattractorsfromnanoscaleexperimentsonanonequilibriumreaction
AT dedeckery reconstructingstochasticattractorsfromnanoscaleexperimentsonanonequilibriumreaction