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

Hossain, Md Jamil; Pawar, Gorakh M.; van Duin, Adri C. T.

doi:10.1149/1945-7111/aca362

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

Journal Article · Thu Nov 24 23:00:00 EST 2022 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/aca362· OSTI ID:1909237

^[1]; ^[2]; van Duin, Adri C. T. ^[3]

Pennsylvania State Univ., University Park, PA (United States); Brown Univ., Providence, RI (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Pennsylvania State Univ., University Park, PA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Laboratory Directed Research and Development (LDRD) Program; US Army Research Laboratory (USARL)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1909237

Report Number(s):: INL/JOU-22-65589-Rev000

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 11 Vol. 169; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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