Elucidating mechanisms of Li plating on Li anodes of lithium-based batteries
Abstract
Lithium metal is known as a very promising anode material for lithium-based batteries possessing a quite high theoretical capacity. But it has been kept away from practical applications due to its extreme reactivity and potential safety hazards led by serious dendrite growth. The origins of dendrite formation may be associated with the mechanisms of Li plating and with the mode of charge transfer during Li reduction or oxidation at the anode-electrolyte interface. Here, density functional theory (DFT) calculations are conducted to analyze the electron transfer between Li (100) and Li cations located in the proximity of the surface in several simulation models. The study includes two common used solvents: ethylene carbonate and dimethoxyethane (EC and DME), and a LiPF6 salt, that surround the Li cation over perfect, defect-containing, and Li2CO3-passivated Li (100) surfaces. Our calculations demonstrate that the Li cation is easily reduced when bonding to DME rather than EC and its preferred deposition site is the hollow site on both perfect and defective Li (100). Additionally, a compact Li2CO3 layer inhibits the charge transfer from Li metal to Li cations, thus modifying Li plating. It is concluded that the extreme reactivity of the Li metal surface induces a stronglymore »
- Authors:
-
- Texas A & M Univ., College Station, TX (United States); Hong Kong University of Science and Technology (HKUST) (Hong Kong)
- Hong Kong University of Science and Technology (HKUST) (Hong Kong)
- Texas A & M Univ., College Station, TX (United States)
- Publication Date:
- Research Org.:
- Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE); Hong Kong University of Science and Technology; Research Grant Council, Hong Kong
- OSTI Identifier:
- 1868846
- Alternate Identifier(s):
- OSTI ID: 1703012; OSTI ID: 1868870
- Grant/Contract Number:
- EE0008210; EE0007766; 26206115; ITS/161/16FP
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Electrochimica Acta
- Additional Journal Information:
- Journal Volume: 284; Journal ID: ISSN 0013-4686
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; density functional theory; lithium electrodeposition; plating; uneven electron distribution; dendritic growth
Citation Formats
Qin, Xueping, Shao, Minhua, and Balbuena, Perla B. Elucidating mechanisms of Li plating on Li anodes of lithium-based batteries. United States: N. p., 2018.
Web. doi:10.1016/j.electacta.2018.07.159.
Qin, Xueping, Shao, Minhua, & Balbuena, Perla B. Elucidating mechanisms of Li plating on Li anodes of lithium-based batteries. United States. https://doi.org/10.1016/j.electacta.2018.07.159
Qin, Xueping, Shao, Minhua, and Balbuena, Perla B. Tue .
"Elucidating mechanisms of Li plating on Li anodes of lithium-based batteries". United States. https://doi.org/10.1016/j.electacta.2018.07.159. https://www.osti.gov/servlets/purl/1868846.
@article{osti_1868846,
title = {Elucidating mechanisms of Li plating on Li anodes of lithium-based batteries},
author = {Qin, Xueping and Shao, Minhua and Balbuena, Perla B.},
abstractNote = {Lithium metal is known as a very promising anode material for lithium-based batteries possessing a quite high theoretical capacity. But it has been kept away from practical applications due to its extreme reactivity and potential safety hazards led by serious dendrite growth. The origins of dendrite formation may be associated with the mechanisms of Li plating and with the mode of charge transfer during Li reduction or oxidation at the anode-electrolyte interface. Here, density functional theory (DFT) calculations are conducted to analyze the electron transfer between Li (100) and Li cations located in the proximity of the surface in several simulation models. The study includes two common used solvents: ethylene carbonate and dimethoxyethane (EC and DME), and a LiPF6 salt, that surround the Li cation over perfect, defect-containing, and Li2CO3-passivated Li (100) surfaces. Our calculations demonstrate that the Li cation is easily reduced when bonding to DME rather than EC and its preferred deposition site is the hollow site on both perfect and defective Li (100). Additionally, a compact Li2CO3 layer inhibits the charge transfer from Li metal to Li cations, thus modifying Li plating. It is concluded that the extreme reactivity of the Li metal surface induces a strongly inhomogeneous electron distribution upon deposition of a cation on the surface. This strong charge inhomogeneity may promote uneven Li nucleation and growth, eventually resulting in dendritic behavior.},
doi = {10.1016/j.electacta.2018.07.159},
journal = {Electrochimica Acta},
number = ,
volume = 284,
place = {United States},
year = {Tue Jul 24 00:00:00 EDT 2018},
month = {Tue Jul 24 00:00:00 EDT 2018}
}
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Works referencing / citing this record:
Density Functional Theory for Battery Materials
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