Display options
Cite
Cheng T, Jaramillo-Botero A, Goddard WA, et al. Adaptive accelerated ReaxFF reactive dynamics with validation from simulating hydrogen combustion. J Am Chem Soc. 2014;136(26):9434-42doi: 10.1021/ja5037258.
Cheng, T., Jaramillo-Botero, A., Goddard, W. A., & Sun, H. (2014). Adaptive accelerated ReaxFF reactive dynamics with validation from simulating hydrogen combustion. Journal of the American Chemical Society, 136(26), 9434-42. https://doi.org/10.1021/ja5037258
Cheng, Tao, et al. "Adaptive accelerated ReaxFF reactive dynamics with validation from simulating hydrogen combustion." Journal of the American Chemical Society vol. 136,26 (2014): 9434-42. doi: https://doi.org/10.1021/ja5037258
Cheng T, Jaramillo-Botero A, Goddard WA, Sun H. Adaptive accelerated ReaxFF reactive dynamics with validation from simulating hydrogen combustion. J Am Chem Soc. 2014 Jul 02;136(26):9434-42. doi: 10.1021/ja5037258. Epub 2014 Jun 23. PMID: 24885152.
Copy Download .nbib Format: NLM
Share it on

J Am Chem Soc. 2014 Jul 02;136(26):9434-42. doi: 10.1021/ja5037258. Epub 2014 Jun 23.

Adaptive accelerated ReaxFF reactive dynamics with validation from simulating hydrogen combustion.

Journal of the American Chemical Society

Tao Cheng, Andrés Jaramillo-Botero, William A Goddard, Huai Sun

Affiliations

  1. School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University , Shanghai 200240, China.

PMID: 24885152 DOI: 10.1021/ja5037258

Abstract

We develop here the methodology for dramatically accelerating the ReaxFF reactive force field based reactive molecular dynamics (RMD) simulations through use of the bond boost concept (BB), which we validate here for describing hydrogen combustion. The bond order, undercoordination, and overcoordination concepts of ReaxFF ensure that the BB correctly adapts to the instantaneous configurations in the reactive system to automatically identify the reactions appropriate to receive the bond boost. We refer to this as adaptive Accelerated ReaxFF Reactive Dynamics or aARRDyn. To validate the aARRDyn methodology, we determined the detailed sequence of reactions for hydrogen combustion with and without the BB. We validate that the kinetics and reaction mechanisms (that is the detailed sequences of reactive intermediates and their subsequent transformation to others) for H2 oxidation obtained from aARRDyn agrees well with the brute force reactive molecular dynamics (BF-RMD) at 2498 K. Using aARRDyn, we then extend our simulations to the whole range of combustion temperatures from ignition (798 K) to flame temperature (2998K), and demonstrate that, over this full temperature range, the reaction rates predicted by aARRDyn agree well with the BF-RMD values, extrapolated to lower temperatures. For the aARRDyn simulation at 798 K we find that the time period for half the H2 to form H2O product is ∼538 s, whereas the computational cost was just 1289 ps, a speed increase of ∼0.42 trillion (10(12)) over BF-RMD. In carrying out these RMD simulations we found that the ReaxFF-COH2008 version of the ReaxFF force field was not accurate for such intermediates as H3O. Consequently we reoptimized the fit to a quantum mechanics (QM) level, leading to the ReaxFF-OH2014 force field that was used in the simulations.

Publication Types