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Nonequilibrium phase coexistence and criticality near the second explosion limit of hydrogen combustion

  • University of Massachusetts Boston

Research output: Contribution to journalArticlepeer-review

Abstract

While hydrogen is a promising source of clean energy, the safety and optimization of hydrogen technologies rely on controlling ignition through explosion limits: pressure-temperature boundaries separating explosive behavior from comparatively slow burning. Here, we show that the emergent nonequilibrium chemistry of combustible mixtures can exhibit the quantitative features of a phase transition. With stochastic simulations of the chemical kinetics for a model mechanism of hydrogen combustion, we show that the boundaries marking explosive domains of kinetic behavior are nonequilibrium critical points. Near the pressure of the second explosion limit, these critical points terminate the transient coexistence of dynamical phases - one that autoignites and another that progresses slowly. Below the critical point temperature, the chemistry of these phases is indistinguishable. In the large system limit, the pseudo-critical temperature converges to the temperature of the second explosion limit derived from mass-action kinetics.

Original languageEnglish
Article number034108
JournalJournal of Chemical Physics
Volume147
Issue number3
DOIs
StatePublished - Jul 21 2017

ASJC Scopus Subject Areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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