In this work, we examine the evolution of events occurring when a Li metal surface is in contact with a 2 M solution of a Li salt in a solvent or mixture of solvents, via classical molecular dynamics simulations with a reactive force field allowing bond breaking and bond forming. The main events include Li oxidation and electrolyte reduction along with expansion of the Li surface layers forming a porous phase that is the basis for the formation of the solid-electrolyte interphase (SEI) components. Nucleation of the main SEI components (LiF, Li oxides, and some organics) is characterized. The analysis clearly reveals the details of these physical–chemical events as a function of time, during 20 nanoseconds. The effects of the chemistry of the electrolyte on Li oxidation and dissolution in the liquid electrolyte, and SEI nucleation and structure are identified by testing two salts: LiPF6 and LiCF3SO3, and various solvents including ethers and carbonates and mixtures of them. The kinetics and thermodynamics of Li6F, the core nuclei in the LiF crystal, are studied by analysis of the MD trajectories, and via density functional theory calculations respectively. The SEI formed in this computational experiment is the “native” film that would form upon contact of the Li foil with the liquid electrolyte. As such, this work is the first in a series of computational experiments that will help elucidate the intricate interphase layer formed during battery cycling using metal anodes.
Ospina-Acevedo, Francisco, et al. "Lithium oxidation and electrolyte decomposition at Li-metal/liquid electrolyte interfaces." Journal of Materials Chemistry. A, vol. 8, no. 33, Jul. 2020. https://doi.org/10.1039/d0ta05132b
Ospina-Acevedo, Francisco, Guo, Ningxuan, & Balbuena, Perla B. (2020). Lithium oxidation and electrolyte decomposition at Li-metal/liquid electrolyte interfaces. Journal of Materials Chemistry. A, 8(33). https://doi.org/10.1039/d0ta05132b
@article{osti_1838784,
author = {Ospina-Acevedo, Francisco and Guo, Ningxuan and Balbuena, Perla B.},
title = {Lithium oxidation and electrolyte decomposition at Li-metal/liquid electrolyte interfaces},
annote = {In this work, we examine the evolution of events occurring when a Li metal surface is in contact with a 2 M solution of a Li salt in a solvent or mixture of solvents, via classical molecular dynamics simulations with a reactive force field allowing bond breaking and bond forming. The main events include Li oxidation and electrolyte reduction along with expansion of the Li surface layers forming a porous phase that is the basis for the formation of the solid-electrolyte interphase (SEI) components. Nucleation of the main SEI components (LiF, Li oxides, and some organics) is characterized. The analysis clearly reveals the details of these physical–chemical events as a function of time, during 20 nanoseconds. The effects of the chemistry of the electrolyte on Li oxidation and dissolution in the liquid electrolyte, and SEI nucleation and structure are identified by testing two salts: LiPF6 and LiCF3SO3, and various solvents including ethers and carbonates and mixtures of them. The kinetics and thermodynamics of Li6F, the core nuclei in the LiF crystal, are studied by analysis of the MD trajectories, and via density functional theory calculations respectively. The SEI formed in this computational experiment is the “native” film that would form upon contact of the Li foil with the liquid electrolyte. As such, this work is the first in a series of computational experiments that will help elucidate the intricate interphase layer formed during battery cycling using metal anodes.},
doi = {10.1039/d0ta05132b},
url = {https://www.osti.gov/biblio/1838784},
journal = {Journal of Materials Chemistry. A},
issn = {ISSN 2050-7488},
number = {33},
volume = {8},
place = {United States},
publisher = {Royal Society of Chemistry},
year = {2020},
month = {07}}
Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
EE0008210
OSTI ID:
1838784
Alternate ID(s):
OSTI ID: 1645156 OSTI ID: 1799458
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 33 Vol. 8; ISSN 2050-7488