Development and application of a ReaxFF reactive force field for hydrogen combustion

Satyam Agrawalla, Adri C.T. Van Duin

Research output: Contribution to journalArticlepeer-review

74 Scopus citations

Abstract

To investigate the reaction kinetics of hydrogen combustion at high-pressure and high-temperature conditions, we constructed a ReaxFF training set to include reaction energies and transition states relevant to hydrogen combustion and optimized the ReaxFF force field parameters against training data obtained from quantum mechanical calculations and experimental values. The optimized ReaxFF potential functions were used to run NVT MD (i.e., molecular dynamics simulation with fixed number of atoms, volume, and temperature) simulations for various H2/O2 mixtures. We observed that the hydroperoxyl (HO2) radical plays a key role in the reaction kinetics at our input conditions (T ≥ 3000 K, P > 400 atm). The reaction mechanism observed is in good agreement with predictions of existing continuum-scale kinetic models for hydrogen combustion, and a transition of reaction mechanism is observed as we move from high pressure, low temperature to low pressure, high temperature. Since ReaxFF derives its parameters from quantum mechanical data and can simulate reaction pathways without any preconditioning, we believe that atomistic simulations through ReaxFF could be a useful tool in enhancing existing continuum-scale kinetic models for prediction of hydrogen combustion kinetics at high-pressure and high-temperature conditions, which otherwise is difficult to attain through experiments.

Original languageEnglish (US)
Pages (from-to)960-972
Number of pages13
JournalJournal of Physical Chemistry A
Volume115
Issue number6
DOIs
StatePublished - Feb 17 2011

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry

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