Theoretical studies on CH4 combustion in O2/H2O atmosphere

Xu Liu; Sitong Yin; Siwei Zhao; Li Yang; Shaozeng Sun; Jiaxu Zhang

doi:10.1016/j.comptc.2021.113199

Theoretical studies on CH₄ combustion in O₂/H₂O atmosphere

Xu Liu
, Sitong Yin
, Siwei Zhao
, Li Yang^*
, Shaozeng Sun
, Jiaxu Zhang

^*Corresponding author for this work

State Key Laboratory of Advanced Welding and Joining
School of Energy Science and Engineering, Harbin Institute of Technology

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

The hydroxyl radical reactions are of extremely significant in combustion chemistry. Direct dynamics simulations are used to study the atomic-level mechanisms of OH(H₂O)_n + CH₄ (n = 0,1,2) reactions starting from the [(H₂O)_nOH—-H—-CH₃] central barrier, which is the important step in the combustion of CH₄ in an O₂/H₂O environment. The simulation results show the propensity for the solvated products due to the thermodynamic preference and the stability of water cluster in products. Although there is a deep minimum (H₂O)_nH₂O—-CH₃ complex in the product exit channel on potential energy surface, the majority of the trajectories avoided this well and instead directly dissociated to products, showing a non-IRC behavior. Significantly, with the addition of two water molecules, the reaction probability, and thus the reaction rate constant increases compared to the one hydrated reaction. This study provides an understanding of CH₄ combustion in O₂/H₂O atmosphere.

Original language	English
Article number	113199
Journal	Computational and Theoretical Chemistry
Volume	1199
DOIs	https://doi.org/10.1016/j.comptc.2021.113199
State	Published - May 2021
Externally published	Yes

Keywords

Combustion reaction
Direct dynamics simulation
Potential energy surface
Solvated reaction

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10.1016/j.comptc.2021.113199

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@article{0e1855297f0e4dbaae3c457d7b7c312f,

title = "Theoretical studies on CH4 combustion in O2/H2O atmosphere",

abstract = "The hydroxyl radical reactions are of extremely significant in combustion chemistry. Direct dynamics simulations are used to study the atomic-level mechanisms of OH(H2O)n + CH4 (n = 0,1,2) reactions starting from the [(H2O)nOH—-H—-CH3] central barrier, which is the important step in the combustion of CH4 in an O2/H2O environment. The simulation results show the propensity for the solvated products due to the thermodynamic preference and the stability of water cluster in products. Although there is a deep minimum (H2O)nH2O—-CH3 complex in the product exit channel on potential energy surface, the majority of the trajectories avoided this well and instead directly dissociated to products, showing a non-IRC behavior. Significantly, with the addition of two water molecules, the reaction probability, and thus the reaction rate constant increases compared to the one hydrated reaction. This study provides an understanding of CH4 combustion in O2/H2O atmosphere.",

keywords = "Combustion reaction, Direct dynamics simulation, Potential energy surface, Solvated reaction",

author = "Xu Liu and Sitong Yin and Siwei Zhao and Li Yang and Shaozeng Sun and Jiaxu Zhang",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

year = "2021",

month = may,

doi = "10.1016/j.comptc.2021.113199",

language = "英语",

volume = "1199",

journal = "Computational and Theoretical Chemistry",

issn = "2210-271X",

publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Theoretical studies on CH4 combustion in O2/H2O atmosphere

AU - Liu, Xu

AU - Yin, Sitong

AU - Zhao, Siwei

AU - Yang, Li

AU - Sun, Shaozeng

AU - Zhang, Jiaxu

PY - 2021/5

Y1 - 2021/5

N2 - The hydroxyl radical reactions are of extremely significant in combustion chemistry. Direct dynamics simulations are used to study the atomic-level mechanisms of OH(H2O)n + CH4 (n = 0,1,2) reactions starting from the [(H2O)nOH—-H—-CH3] central barrier, which is the important step in the combustion of CH4 in an O2/H2O environment. The simulation results show the propensity for the solvated products due to the thermodynamic preference and the stability of water cluster in products. Although there is a deep minimum (H2O)nH2O—-CH3 complex in the product exit channel on potential energy surface, the majority of the trajectories avoided this well and instead directly dissociated to products, showing a non-IRC behavior. Significantly, with the addition of two water molecules, the reaction probability, and thus the reaction rate constant increases compared to the one hydrated reaction. This study provides an understanding of CH4 combustion in O2/H2O atmosphere.

AB - The hydroxyl radical reactions are of extremely significant in combustion chemistry. Direct dynamics simulations are used to study the atomic-level mechanisms of OH(H2O)n + CH4 (n = 0,1,2) reactions starting from the [(H2O)nOH—-H—-CH3] central barrier, which is the important step in the combustion of CH4 in an O2/H2O environment. The simulation results show the propensity for the solvated products due to the thermodynamic preference and the stability of water cluster in products. Although there is a deep minimum (H2O)nH2O—-CH3 complex in the product exit channel on potential energy surface, the majority of the trajectories avoided this well and instead directly dissociated to products, showing a non-IRC behavior. Significantly, with the addition of two water molecules, the reaction probability, and thus the reaction rate constant increases compared to the one hydrated reaction. This study provides an understanding of CH4 combustion in O2/H2O atmosphere.

KW - Combustion reaction

KW - Direct dynamics simulation

KW - Potential energy surface

KW - Solvated reaction

UR - https://www.scopus.com/pages/publications/85103266976

U2 - 10.1016/j.comptc.2021.113199

DO - 10.1016/j.comptc.2021.113199

M3 - 文章

AN - SCOPUS:85103266976

SN - 2210-271X

VL - 1199

JO - Computational and Theoretical Chemistry

JF - Computational and Theoretical Chemistry

M1 - 113199

ER -

Theoretical studies on CH₄ combustion in O₂/H₂O atmosphere

Abstract

Keywords

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