Reactive force field simulation studies on the combustion behavior of n -octanol

Bharti, Anand Kumar; Banerjee, Tamal

doi:10.1016/j.fuproc.2016.06.027

Cited by 39 publications

(20 citation statements)

References 29 publications

(38 reference statements)

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“…The CHO-2008 pararametrization has been applied to various systems. [66][67][68][69][70][71][72][73][74] For all these cases, "generally a good agreement with experimental results in terms of the initiation mechanism and barriers were observed". [52] Comparison of the bond dissociation energies of the species used in the training data (ReaxFF bond dissociation energies vs. B3LYP bond dissociation energies, cf.…”

Section: Methodssupporting

confidence: 54%

“…We chose the well‐established CHO‐2008 parametrization by Chenoweth et al., which has been designed to study combustion processes. The CHO‐2008 pararametrization has been applied to various systems . For all these cases, “generally a good agreement with experimental results in terms of the initiation mechanism and barriers were observed” .…”

Section: Methodsmentioning

confidence: 55%

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Exploring the Chemistry of Low‐Temperature Ignition by Pressure‐Accelerated Dynamics

et al. 2020

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Reaction models that accurately describe the complex reaction processes of ignition are key for the development of novel engine-and fuel concepts. Since reactive molecular dynamics can be used to discover reaction networks in a largely automated fashion, this method has the potential to drastically reduce the real time effort necessary for the development of reaction models. With standard reactive molecular dynamics, the simulation of low-temperature reaction processes is hindered by the small accessible time scales of only a few nanoseconds. In this work, we propose the pressure-accelerated dynamics method to overcome the time scales obstacle through exploitation of Le Chatelier's principle. For the example of pentane low-temperature ignition, we show that with pressure-accelerated dynamics, the ReaxFF reactive force field, and the ChemTraYzer not only the known key low-temperature igniton pathways can be found, but also reactions that are not yet included in reaction models.

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Section: Methodssupporting

confidence: 54%

Section: Methodsmentioning

confidence: 55%

Exploring the Chemistry of Low‐Temperature Ignition by Pressure‐Accelerated Dynamics

et al. 2020

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“…While these results appear to be a condemnation of ReaxFF methods for these systems, studies by both the developers 39,[51][52][53][54][55]57,58,61,63,[67][68][69][70][71][72]74,[76][77][78][79][80][81][83][84][85][86][87][88][89][90][91][92][93][94][95][96][97] and users [31][32][33][34]56,59,60,62,[64][65][66]73,75,…”

Section: Intrinsic Reaction Coordinate Scansmentioning

confidence: 99%

Benchmarking the Performance of the ReaxFF Reactive Force Field on Hydrogen Combustion Systems

et al. 2020

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A thorough understanding of the kinetics and dynamics of combusting mixtures is of considerable interest, especially in regimes beyond the reach of current experimental validation. The ReaxFF reactive force field method has provided a way to simulate large-scale systems of hydrogen combustion via a parameterized potential that can simulate bond breaking. This modeling approach has been applied to hydrogen combustion, as well as myriad other reactive chemical systems. In this work, we benchmark the performance of several common parameterizations of this potential against higherlevel quantum mechanical (QM) approaches. We demonstrate instances where these parameterizations of the ReaxFF potential fail both quantitatively and qualitatively to describe reactive events relevant for hydrogen combustion systems.

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“…As the training set did not have data for any highly strained aliphatic molecule like JP-10, it clearly demonstrated the transferability of the ReaxFF CHO-2008 description in studying different hydrocarbon fuels. Since then it has been implemented in a wide range of applications in the scientific community for studying pyrolysis and oxidation of variety of fuels. − ,,− These parameter sets are further extended to other elements including nitrogen/boron and various transition metals, which makes it a highly versatile atomistic-scale tool to study combustion dynamics. Thus, over the past few years, the ReaxFF CHO-2008 description has been used to study the pyrolysis and combustion of n -dodecane, 1-heptane, n -octanol, toluene, Illinois No.…”

Section: Introductionmentioning

confidence: 99%

“…Since then it has been implemented in a wide range of applications in the scientific community for studying pyrolysis and oxidation of variety of fuels. − ,,− These parameter sets are further extended to other elements including nitrogen/boron and various transition metals, which makes it a highly versatile atomistic-scale tool to study combustion dynamics. Thus, over the past few years, the ReaxFF CHO-2008 description has been used to study the pyrolysis and combustion of n -dodecane, 1-heptane, n -octanol, toluene, Illinois No. 6 coal, 1,6-dicyclopropane-2,4-hexyne, and liginin .…”

Section: Introductionmentioning

confidence: 99%

Extension of the ReaxFF Combustion Force Field toward Syngas Combustion and Initial Oxidation Kinetics

2017

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A detailed insight of key reactive events related to oxidation and pyrolysis of hydrocarbon fuels further enhances our understanding of combustion chemistry. Though comprehensive kinetic models are available for smaller hydrocarbons (typically C or lower), developing and validating reaction mechanisms for larger hydrocarbons is a daunting task, due to the complexity of their reaction networks. The ReaxFF method provides an attractive computational method to obtain reaction kinetics for complex fuel and fuel mixtures, providing an accuracy approaching ab-initio-based methods but with a significantly lower computational expense. The development of the first ReaxFF combustion force field by Chenoweth et al. (CHO-2008 parameter set) in 2008 has opened new avenues for researchers to investigate combustion chemistry from the atomistic level. In this article, we seek to address two issues with the CHO-2008 ReaxFF description. While the CHO-2008 description has achieved significant popularity for studying large hydrocarbon combustion, it fails to accurately describe the chemistry of small hydrocarbon oxidation, especially conversion of CO from CO, which is highly relevant to syngas combustion. Additionally, the CHO-2008 description was obtained faster than expected H abstraction by O from hydrocarbons, thus underestimating the oxidation initiation temperature. In this study, we seek to systemically improve the CHO-2008 description and validate it for these cases. Additionally, our aim was to retain the accuracy of the 2008 description for larger hydrocarbons and provide similar quality results. Thus, we expanded the ReaxFF CHO-2008 DFT-based training set by including reactions and transition state structures relevant to the syngas and oxidation initiation pathways and retrained the parameters. To validate the quality of our force field, we performed high-temperature NVT-MD simulations to study oxidation and pyrolysis of four different hydrocarbon fuels, namely, syngas, methane, JP-10, and n-butylbenzene. Results obtained from syngas and methane oxidation simulation indicated that our redeveloped parameters (named as the CHO-2016 parameter set) has significantly improved the C chemistry predicted by ReaxFF and has solved the low-temperature oxidation initiation problem. Moreover, Arrhenius parameters of JP-10 decomposition and initiation mechanism pathways of n-butylbenzene pyrolysis obtained using the CHO-2016 parameter set are also in good agreement with both experimental and CHO-2008 simulation results. This demonstrated the transferability of the CHO-2016 description for a wide range of hydrocarbon chemistry.

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Reactive force field simulation studies on the combustion behavior of n -octanol

Cited by 39 publications

References 29 publications

Exploring the Chemistry of Low‐Temperature Ignition by Pressure‐Accelerated Dynamics

Exploring the Chemistry of Low‐Temperature Ignition by Pressure‐Accelerated Dynamics

Benchmarking the Performance of the ReaxFF Reactive Force Field on Hydrogen Combustion Systems

Extension of the ReaxFF Combustion Force Field toward Syngas Combustion and Initial Oxidation Kinetics

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