First-principles-based reaction kinetics from reactive molecular dynamics simulations: Application to hydrogen peroxide decomposition

Proceedings of the National Academy of Sciences of the United States of America
Daniil V IlyinTao Cheng

Abstract

This paper presents our vision of how to use in silico approaches to extract the reaction mechanisms and kinetic parameters for complex condensed-phase chemical processes that underlie important technologies ranging from combustion to chemical vapor deposition. The goal is to provide an analytic description of the detailed evolution of a complex chemical system from reactants through various intermediates to products, so that one could optimize the efficiency of the reactive processes to produce the desired products and avoid unwanted side products. We could start with quantum mechanics (QM) to ensure an accurate description; however, to obtain useful kinetics we need to average over ∼10-nm spatial scales for ∼1 ns, which is prohibitively impractical with QM. Instead, we use the reactive force field (ReaxFF) trained to fit QM to carry out the reactive molecular dynamics (RMD). We focus here on showing that it is practical to extract from such RMD the reaction mechanisms and kinetics information needed to describe the reactions analytically. This analytic description can then be used to incorporate the correct reaction chemistry from the QM/ReaxFF atomistic description into larger-scale simulations of ∼10 nm to micrometers to mi...Continue Reading

References

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Citations

Aug 8, 2018·Proceedings of the National Academy of Sciences of the United States of America·Snezhana I AbarzhiSergei I Anisimov
Sep 11, 2019·Proceedings of the National Academy of Sciences of the United States of America·Snezhana I Abarzhi, William A Goddard
Feb 12, 2021·The Journal of Physical Chemistry. a·Jason FordTodd J Martínez
May 27, 2021·Nature Communications·Matthew J McDermottKristin A Persson

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