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Title: An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics

Abstract

We report a novel atomistic model of carbide-derived carbons (CDCs), which are nanoporous carbons with high specific surface areas, synthesis-dependent degrees of graphitization, and well-ordered, tunable porosities. These properties make CDCs viable substrates in several energy-relevant applications, such as gas storage media, electrochemical capacitors, and catalytic supports. These materials are heterogenous, non-ideal structures and include several important parameters that govern their performance. Therefore, a realistic model of the CDC structure is needed in order to study these systems and their nanoscale and macroscale properties with molecular simulation. We report the use of the ReaxFF reactive force field in a quenched molecular dynamics routine to generate atomistic CDC models. The pair distribution function, pore size distribution, and adsorptive properties of this model are reported and corroborated with experimental data. Simulations demonstrate that compressing the system after quenching changes the pore size distribution to better match the experimental target. Ring size distributions of this model demonstrate the prevalence of non-hexagonal carbon rings in CDCs. Furthermore, these effects may contrast the properties of CDCs against those of activated carbons with similar pore size distributions and explain higher energy densities of CDC-based supercapacitors.

Authors:
 [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [5]; ORCiD logo [5];  [1];  [2];  [6];  [1]
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Drexel Univ., Philadelphia, PA (United States)
  3. The Univ. of Tennessee/Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Alabama, Tuscaloosa, AL (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. The Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1468248
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
C
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2311-5629
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanoporous carbon; carbide-derived carbon; reactive molecular dynamics

Citation Formats

Thompson, Matthew W., Dyatkin, Boris, Wang, Hsiu -Wen, Turner, C. Heath, Sang, Xiahan, Unocic, Raymond R., Iacovella, Christopher R., Gogotsi, Yury, van Duin, Adri C. T., and Cummings, Peter T. An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics. United States: N. p., 2017. Web. doi:10.3390/c3040032.
Thompson, Matthew W., Dyatkin, Boris, Wang, Hsiu -Wen, Turner, C. Heath, Sang, Xiahan, Unocic, Raymond R., Iacovella, Christopher R., Gogotsi, Yury, van Duin, Adri C. T., & Cummings, Peter T. An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics. United States. doi:10.3390/c3040032.
Thompson, Matthew W., Dyatkin, Boris, Wang, Hsiu -Wen, Turner, C. Heath, Sang, Xiahan, Unocic, Raymond R., Iacovella, Christopher R., Gogotsi, Yury, van Duin, Adri C. T., and Cummings, Peter T. Mon . "An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics". United States. doi:10.3390/c3040032. https://www.osti.gov/servlets/purl/1468248.
@article{osti_1468248,
title = {An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics},
author = {Thompson, Matthew W. and Dyatkin, Boris and Wang, Hsiu -Wen and Turner, C. Heath and Sang, Xiahan and Unocic, Raymond R. and Iacovella, Christopher R. and Gogotsi, Yury and van Duin, Adri C. T. and Cummings, Peter T.},
abstractNote = {We report a novel atomistic model of carbide-derived carbons (CDCs), which are nanoporous carbons with high specific surface areas, synthesis-dependent degrees of graphitization, and well-ordered, tunable porosities. These properties make CDCs viable substrates in several energy-relevant applications, such as gas storage media, electrochemical capacitors, and catalytic supports. These materials are heterogenous, non-ideal structures and include several important parameters that govern their performance. Therefore, a realistic model of the CDC structure is needed in order to study these systems and their nanoscale and macroscale properties with molecular simulation. We report the use of the ReaxFF reactive force field in a quenched molecular dynamics routine to generate atomistic CDC models. The pair distribution function, pore size distribution, and adsorptive properties of this model are reported and corroborated with experimental data. Simulations demonstrate that compressing the system after quenching changes the pore size distribution to better match the experimental target. Ring size distributions of this model demonstrate the prevalence of non-hexagonal carbon rings in CDCs. Furthermore, these effects may contrast the properties of CDCs against those of activated carbons with similar pore size distributions and explain higher energy densities of CDC-based supercapacitors.},
doi = {10.3390/c3040032},
journal = {C},
number = 4,
volume = 3,
place = {United States},
year = {2017},
month = {10}
}

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