Molecular model and ReaxFF molecular dynamics simulation of coal vitrinite pyrolysis

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• 作者：Wu Li ; Yan-ming Zhu ; Geoff Wang ; Yang Wang ; Yu Liu
• 关键词：Coal ; Molecular model ; Pyrolysis ; ReaxFF molecular dynamics ; Vitrinite
• 刊名：Journal of Molecular Modeling
• 出版年：2015
• 出版时间：August 2015
• 年：2015
• 卷：21
• 期：8
• 全文大小：2,790 KB
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• 作者单位：Wu Li (1) (2)
  Yan-ming Zhu (1)
  Geoff Wang (2)
  Yang Wang (1)
  Yu Liu (1)
  
  1. Key Laboratory of Coalbed Methane Resource & Reservoir Formation Process, Ministry of Education, China University of Mining & Technology, Xuzhou, 221116, People’s Republic of China
  2. School of Chemical Engineering, The University of Queensland, St. Lucia, Brisbane, QLD, 4072, Australia
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Computer Applications in Chemistry
  Biomedicine
  Molecular Medicine
  Health Informatics and Administration
  Life Sciences
  Computer Application in Life Sciences
  
• 出版者：Springer Berlin / Heidelberg
• ISSN：0948-5023

文摘

Vitrinite in coal, the mainly generating methane maceral, plays an important role in hydrocarbon generation of coal. This study aims at obtaining products formation mechanism of vitrinite pyrolysis, and hence determining the chemical bond, molecular liquefaction activity, and reactions mechanism of methane and C2- during pyrolysis. The ReaxFF molecular dynamics (MD) simulation was carried out at temperature of 1500?K in order to investigate the mechanism of vitrinite pyrolysis. Initially, a minimum energy conformational structure model was constrained by a combination of elemental and carbon-13 nuclear magnetic resonance (13C NMR) literature data. The model analysis shows the chemical and physical parameters of vitrinite pyrolysis are broadly consistent with the experimental data. Based on the molecular model, ReaxFF MD simulations further provide information of unimolecule such as bond length, and chemical shift, and hence the total population and energy of main products. Molecules bond and pyrolysis fragments, based on active bond analyzed, revealed pyrolysis products of single vitrinite molecule with aliphatic C-C bond, especially ring and chain aliphatic as liquefaction activity. The molecular cell whose density is 0.9?g/cm3 with lowest energy accords with the experimental density 1.33?g/cm3. The content of main products after pyrolysis, classifying as CH4, H2O, and H2, was changed along with the increasing temperature. The gas molecule, fragments and generation pathways of CO2, H2, CH4, and C2H6 were also elucidated. These results show agreement with experimental observations, implying that MD simulation can provide reasonable explanation for the reaction processes involved in coal vitrinite pyrolysis. Thus the mechanism of coal hydrocarbon generation was revealed at the molecular level.