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Title: Development and Applications of an eReaxFF Force Field for Graphitic Anodes of Lithium-Ion Batteries

Abstract

Graphene is one of the most promising materials for lithium-ion battery anodes due to its superior electronic conductivity, high surface area for lithium intercalation, fast ionic diffusivity and enhanced specific capacity. A reliable description of many battery processes requires an explicit description of electrochemical interactions involving electrons. A detailed atomistic modeling of electronic conduction and non-zero voltage simulations of graphitic materials require the inclusion of an explicit electronic degree of freedom. To enable large length- and time-scale simulations of electron conduction in graphitic anodes, we developed an eReaxFF force field concept describing graphitic materials with an explicit electron. The newly developed force field, verified against quantum chemistry-based data describing, amongst others, electron affinities and equation of states, reproduces the qualitative behavior of electron conductivity in pristine and imperfect graphitic materials at different applied temperatures and voltages. In addition, excess electron localization near a defect site estimated from eReaxFF simulations agree quite well with the corresponding density functional theory calculations. Here, our eReaxFF simulations show the initiation of lithium-metal-plating driven by electron transfer from the graphene surface to the exposed lithium ions demonstrating the method’s potential for studying lithium-graphene interactions with explicit electrons and explain many unresolved electrode and electrode-electrolyte interfacemore » processes.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]
+ Show Author Affiliations
  1. Pennsylvania State Univ., University Park, PA (United States); Brown Univ., Providence, RI (United States)
  2. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  3. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); USDOE Laboratory Directed Research and Development (LDRD) Program; US Army Research Laboratory (USARL)
OSTI Identifier:
1909237
Report Number(s):
INL/JOU-22-65589-Rev000
Journal ID: ISSN 0013-4651; TRN: US2312107
Grant/Contract Number:  
AC07-05ID14517; W911NF-12-2-0023
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 169; Journal Issue: 11; Journal ID: ISSN 0013-4651
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Molecular Dynamics Simulation; Electron; Graphite

Citation Formats

Hossain, Md Jamil, Pawar, Gorakh M., and van Duin, Adri C. T. Development and Applications of an eReaxFF Force Field for Graphitic Anodes of Lithium-Ion Batteries. United States: N. p., 2022. Web. doi:10.1149/1945-7111/aca362.
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Hossain, Md Jamil, Pawar, Gorakh M., & van Duin, Adri C. T. Development and Applications of an eReaxFF Force Field for Graphitic Anodes of Lithium-Ion Batteries. United States. https://doi.org/10.1149/1945-7111/aca362
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Hossain, Md Jamil, Pawar, Gorakh M., and van Duin, Adri C. T. Fri . "Development and Applications of an eReaxFF Force Field for Graphitic Anodes of Lithium-Ion Batteries". United States. https://doi.org/10.1149/1945-7111/aca362. https://www.osti.gov/servlets/purl/1909237.
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@article{osti_1909237,
title = {Development and Applications of an eReaxFF Force Field for Graphitic Anodes of Lithium-Ion Batteries},
author = {Hossain, Md Jamil and Pawar, Gorakh M. and van Duin, Adri C. T.},
abstractNote = {Graphene is one of the most promising materials for lithium-ion battery anodes due to its superior electronic conductivity, high surface area for lithium intercalation, fast ionic diffusivity and enhanced specific capacity. A reliable description of many battery processes requires an explicit description of electrochemical interactions involving electrons. A detailed atomistic modeling of electronic conduction and non-zero voltage simulations of graphitic materials require the inclusion of an explicit electronic degree of freedom. To enable large length- and time-scale simulations of electron conduction in graphitic anodes, we developed an eReaxFF force field concept describing graphitic materials with an explicit electron. The newly developed force field, verified against quantum chemistry-based data describing, amongst others, electron affinities and equation of states, reproduces the qualitative behavior of electron conductivity in pristine and imperfect graphitic materials at different applied temperatures and voltages. In addition, excess electron localization near a defect site estimated from eReaxFF simulations agree quite well with the corresponding density functional theory calculations. Here, our eReaxFF simulations show the initiation of lithium-metal-plating driven by electron transfer from the graphene surface to the exposed lithium ions demonstrating the method’s potential for studying lithium-graphene interactions with explicit electrons and explain many unresolved electrode and electrode-electrolyte interface processes.},
doi = {10.1149/1945-7111/aca362},
journal = {Journal of the Electrochemical Society},
number = 11,
volume = 169,
place = {United States},
year = {Fri Nov 25 00:00:00 EST 2022},
month = {Fri Nov 25 00:00:00 EST 2022}
}
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