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Title: Reactive Molecular Dynamics Simulation of Kerogen Thermal Maturation and Cross-Linking Pathways

For this study, molecular dynamics simulations were performed with a ReaxFF reactive force field to investigate bond breaking and bond formation mechanisms during the early thermal maturation of kerogen and potential crosslinking pathways towards a three-dimensional (3D) quasi-infinite molecular network (crosslinked kerogen). Starting with small ensembles of high molecular mass models for immature type I Green River Shale kerogen (Kerogen 1-I), top of the oil window type II kerogen (Kerogen 2-L), and low maturity type III kerogen (Kerogen 3-L), low molecular mass species including H 2O, H 2S, C 2H 4, C 3H 6 were produced as the maturities of the remaining kerogens increased. Highly reactive fragments, which are not detected in pyrolysis experiments, were also produced. Further, the crosslinking mechanism in the newly develop polymeric kerogen networks appears to be highly complex and it is influenced by the nature of the kerogen. Covalent —C—S—, —C—O— and —C—C— bonds are the primary crosslinks that structurally binds kerogen monomers together. The trends observed in the thermochemical transformation of kerogen and the kerogen crosslinking pathways are consistent with the theoretical and experimental studies reported in the scientific literature. The reactive force field molecular dynamics simulation provides a potentially valuable alternative approach tomore » the development of a realistic 3D molecular network of kerogen. However, the conversion of kerogen molecules into a 3D molecular network was low.« less
Authors:
ORCiD logo [1] ;  [2] ;  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Temple Univ., Philadelphia, PA (United States)
Publication Date:
Report Number(s):
INL/JOU-17-41419
Journal ID: ISSN 0887-0624
Grant/Contract Number:
AC07-05ID14517
Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 31; Journal Issue: 11; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Research Org:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE); USDOE Laboratory Directed Research and Development (LDRD) Program
Contributing Orgs:
Boise State Univ., ID (United States); Pennsylvania State Univ., University Park, PA (United States)
Country of Publication:
United States
Language:
English
Subject:
04 OIL SHALES AND TAR SANDS; 02 PETROLEUM; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Kerogen Crosslinking; Reactive Molecular Dynamics
OSTI Identifier:
1414450

Pawar, Gorakh, Meakin, Paul, and Huang, Hai. Reactive Molecular Dynamics Simulation of Kerogen Thermal Maturation and Cross-Linking Pathways. United States: N. p., Web. doi:10.1021/acs.energyfuels.7b01555.
Pawar, Gorakh, Meakin, Paul, & Huang, Hai. Reactive Molecular Dynamics Simulation of Kerogen Thermal Maturation and Cross-Linking Pathways. United States. doi:10.1021/acs.energyfuels.7b01555.
Pawar, Gorakh, Meakin, Paul, and Huang, Hai. 2017. "Reactive Molecular Dynamics Simulation of Kerogen Thermal Maturation and Cross-Linking Pathways". United States. doi:10.1021/acs.energyfuels.7b01555. https://www.osti.gov/servlets/purl/1414450.
@article{osti_1414450,
title = {Reactive Molecular Dynamics Simulation of Kerogen Thermal Maturation and Cross-Linking Pathways},
author = {Pawar, Gorakh and Meakin, Paul and Huang, Hai},
abstractNote = {For this study, molecular dynamics simulations were performed with a ReaxFF reactive force field to investigate bond breaking and bond formation mechanisms during the early thermal maturation of kerogen and potential crosslinking pathways towards a three-dimensional (3D) quasi-infinite molecular network (crosslinked kerogen). Starting with small ensembles of high molecular mass models for immature type I Green River Shale kerogen (Kerogen 1-I), top of the oil window type II kerogen (Kerogen 2-L), and low maturity type III kerogen (Kerogen 3-L), low molecular mass species including H2O, H2S, C2H4, C3H6 were produced as the maturities of the remaining kerogens increased. Highly reactive fragments, which are not detected in pyrolysis experiments, were also produced. Further, the crosslinking mechanism in the newly develop polymeric kerogen networks appears to be highly complex and it is influenced by the nature of the kerogen. Covalent —C—S—, —C—O— and —C—C— bonds are the primary crosslinks that structurally binds kerogen monomers together. The trends observed in the thermochemical transformation of kerogen and the kerogen crosslinking pathways are consistent with the theoretical and experimental studies reported in the scientific literature. The reactive force field molecular dynamics simulation provides a potentially valuable alternative approach to the development of a realistic 3D molecular network of kerogen. However, the conversion of kerogen molecules into a 3D molecular network was low.},
doi = {10.1021/acs.energyfuels.7b01555},
journal = {Energy and Fuels},
number = 11,
volume = 31,
place = {United States},
year = {2017},
month = {9}
}