Dendrite formation in Li-metal anodes: an atomistic molecular dynamics study
Abstract
Lithium-metal is a desired material for anodes of Li-ion and beyond Li-ion batteries because of its large theoretical specific capacity of 3860 mA h g-1 (the highest known so far), low density, and extremely low potential. Unfortunately, there are several problems that restrict the practical application of lithium-metal anodes, such as the formation of dendrites and reactivity with electrolytes. We present here a study of lithium dendrite formation on a Li-metal anode covered by a cracked solid electrolyte interface (SEI) of LiF in contact with a typical liquid electrolyte composed of 1 M LiPF6 salt solvated in ethylene carbonate. The study uses classical molecular dynamics on a model nanobattery. We tested three ways to charge the nanobattery: (1) constant current at a rate of one Li+ per 0.4 ps, (2) pulse train 10 Li+ per 4 ps, and (3) constant number ions in the electrolyte: one Li+ enters the electrolyte from the cathode as one Li+ exits the electrolyte to the anode. We found that although the SEI does not interfere with the lithiation, the mere presence of a crack in the SEI boosts and guides dendrite formation at temperatures between 325 K and 410.7 K at any C-rate, beingmore »
- Authors:
-
- Department of Chemical Engineering, Department of Electrical and Computer Engineering, Department of Materials Science and Engineering, Texas A&M University, College Station
- 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)
- OSTI Identifier:
- 1560276
- Alternate Identifier(s):
- OSTI ID: 1614098
- Grant/Contract Number:
- EE0008210
- Resource Type:
- Published Article
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Name: RSC Advances Journal Volume: 9 Journal Issue: 48; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry
Citation Formats
Selis, Luis A., and Seminario, Jorge M.. Dendrite formation in Li-metal anodes: an atomistic molecular dynamics study. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9RA05067A.
Selis, Luis A., & Seminario, Jorge M.. Dendrite formation in Li-metal anodes: an atomistic molecular dynamics study. United Kingdom. https://doi.org/10.1039/C9RA05067A
Selis, Luis A., and Seminario, Jorge M.. Wed .
"Dendrite formation in Li-metal anodes: an atomistic molecular dynamics study". United Kingdom. https://doi.org/10.1039/C9RA05067A.
@article{osti_1560276,
title = {Dendrite formation in Li-metal anodes: an atomistic molecular dynamics study},
author = {Selis, Luis A. and Seminario, Jorge M.},
abstractNote = {Lithium-metal is a desired material for anodes of Li-ion and beyond Li-ion batteries because of its large theoretical specific capacity of 3860 mA h g-1 (the highest known so far), low density, and extremely low potential. Unfortunately, there are several problems that restrict the practical application of lithium-metal anodes, such as the formation of dendrites and reactivity with electrolytes. We present here a study of lithium dendrite formation on a Li-metal anode covered by a cracked solid electrolyte interface (SEI) of LiF in contact with a typical liquid electrolyte composed of 1 M LiPF6 salt solvated in ethylene carbonate. The study uses classical molecular dynamics on a model nanobattery. We tested three ways to charge the nanobattery: (1) constant current at a rate of one Li+ per 0.4 ps, (2) pulse train 10 Li+ per 4 ps, and (3) constant number ions in the electrolyte: one Li+ enters the electrolyte from the cathode as one Li+ exits the electrolyte to the anode. We found that although the SEI does not interfere with the lithiation, the mere presence of a crack in the SEI boosts and guides dendrite formation at temperatures between 325 K and 410.7 K at any C-rate, being more favorable at 325 K than at 410.7 K. On the other hand, we find that a higher C-rate (2.2C) favors the lithium dendrite formation compared to a lower C-rate (1.6C). Thus the battery could store more energy in a safe way at a lower C-rate.},
doi = {10.1039/C9RA05067A},
journal = {RSC Advances},
number = 48,
volume = 9,
place = {United Kingdom},
year = {2019},
month = {9}
}
https://doi.org/10.1039/C9RA05067A
Web of Science
Works referenced in this record:
Effect of electrolytes on the structure and evolution of the solid electrolyte interphase (SEI) in Li-ion batteries: A molecular dynamics study
journal, October 2011
- Kim, Sang-Pil; Duin, Adri C. T. van; Shenoy, Vivek B.
- Journal of Power Sources, Vol. 196, Issue 20
Dendrite formation in silicon anodes of lithium-ion batteries
journal, January 2018
- Selis, Luis A.; Seminario, Jorge M.
- RSC Advances, Vol. 8, Issue 10
In-Situ Observations of Lithium Dendrite Growth
journal, January 2018
- Kong, Lingxi; Xing, Yinjiao; Pecht, Michael G.
- IEEE Access, Vol. 6
UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992
- Rappe, A. K.; Casewit, C. J.; Colwell, K. S.
- Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035
Deciphering the multi-step degradation mechanisms of carbonate-based electrolyte in Li batteries
journal, March 2008
- Gachot, Gregory; Grugeon, Sylvie; Armand, Michel
- Journal of Power Sources, Vol. 178, Issue 1
Reductive Decomposition Reactions of Ethylene Carbonate by Explicit Electron Transfer from Lithium: An eReaxFF Molecular Dynamics Study
journal, November 2016
- Islam, Md Mahbubul; van Duin, Adri C. T.
- The Journal of Physical Chemistry C, Vol. 120, Issue 48
Towards superior volumetric performance: design and preparation of novel carbon materials for energy storage
journal, January 2015
- Zhang, Chen; Lv, Wei; Tao, Ying
- Energy & Environmental Science, Vol. 8, Issue 5
Observation of Lithium Dendrites at Ambient Temperature and Below
journal, December 2014
- Love, C. T.; Baturina, O. A.; Swider-Lyons, K. E.
- ECS Electrochemistry Letters, Vol. 4, Issue 2
Lithium Diffusion Mechanism through Solid–Electrolyte Interphase in Rechargeable Lithium Batteries
journal, March 2019
- Ramasubramanian, Ajaykrishna; Yurkiv, Vitaliy; Foroozan, Tara
- The Journal of Physical Chemistry C, Vol. 123, Issue 16
Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies
journal, January 2017
- Barai, Pallab; Higa, Kenneth; Srinivasan, Venkat
- Physical Chemistry Chemical Physics, Vol. 19, Issue 31
Dielectric properties and relaxation in ethylene carbonate and propylene carbonate
journal, September 1972
- Payne, Richard; Theodorou, Ignatius E.
- The Journal of Physical Chemistry, Vol. 76, Issue 20
Lithium dendrite growth mechanisms in liquid electrolytes
journal, November 2017
- Jana, Aniruddha; García, R. Edwin
- Nano Energy, Vol. 41
Factors Which Limit the Cycle Life of Rechargeable Lithium (Metal) Batteries
journal, January 2000
- Aurbach, D.; Zinigrad, E.; Teller, H.
- Journal of The Electrochemical Society, Vol. 147, Issue 4
Modeling the potential impact of lithium recycling from EV batteries on lithium demand: A dynamic MFA approach
journal, June 2018
- Ziemann, Saskia; Müller, Daniel B.; Schebek, Liselotte
- Resources, Conservation and Recycling, Vol. 133
Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995
- Plimpton, Steve
- Journal of Computational Physics, Vol. 117, Issue 1
Highly Stable Lithium Metal Batteries Enabled by Regulating the Solvation of Lithium Ions in Nonaqueous Electrolytes
journal, March 2018
- Zhang, Xue-Qiang; Chen, Xiang; Cheng, Xin-Bing
- Angewandte Chemie International Edition, Vol. 57, Issue 19
Protected Lithium-Metal Anodes in Batteries: From Liquid to Solid
journal, July 2017
- Yang, Chunpeng; Fu, Kun; Zhang, Ying
- Advanced Materials, Vol. 29, Issue 36
Suppression of Lithium Dendrite Formation by Using LAGP-PEO (LiTFSI) Composite Solid Electrolyte and Lithium Metal Anode Modified by PEO (LiTFSI) in All-Solid-State Lithium Batteries
journal, April 2017
- Wang, Chunhua; Yang, Yifu; Liu, Xingjiang
- ACS Applied Materials & Interfaces, Vol. 9, Issue 15
Molecular dynamics simulation of diffusion and viscosity of liquid lithium fluoride
journal, January 2016
- Luo, Hui; Xiao, Shifang; Wang, Shengjie
- Computational Materials Science, Vol. 111
Dielectric Constant, Dipole Moment, and Solubility Parameters of Some Cyclic Acid Esters
journal, March 2006
- Chernyak, Yury
- Journal of Chemical & Engineering Data, Vol. 51, Issue 2
Electronegativity-equalization method for the calculation of atomic charges in molecules
journal, July 1986
- Mortier, Wilfried J.; Ghosh, Swapan K.; Shankar, S.
- Journal of the American Chemical Society, Vol. 108, Issue 15
Lithium metal anodes for rechargeable batteries
journal, January 2014
- Xu, Wu; Wang, Jiulin; Ding, Fei
- Energy Environ. Sci., Vol. 7, Issue 2
A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984
- Nosé, Shuichi
- The Journal of Chemical Physics, Vol. 81, Issue 1
Transition of lithium growth mechanisms in liquid electrolytes
journal, January 2016
- Bai, Peng; Li, Ju; Brushett, Fikile R.
- Energy & Environmental Science, Vol. 9, Issue 10
Interconnected hollow carbon nanospheres for stable lithium metal anodes
journal, July 2014
- Zheng, Guangyuan; Lee, Seok Woo; Liang, Zheng
- Nature Nanotechnology, Vol. 9, Issue 8
Reactions of Singly-Reduced Ethylene Carbonate in Lithium Battery Electrolytes: A Molecular Dynamics Simulation Study Using the ReaxFF
journal, December 2011
- Bedrov, Dmitry; Smith, Grant D.; van Duin, Adri C. T.
- The Journal of Physical Chemistry A, Vol. 116, Issue 11
Implementing molecular dynamics on hybrid high performance computers – Particle–particle particle-mesh
journal, March 2012
- Brown, W. Michael; Kohlmeyer, Axel; Plimpton, Steven J.
- Computer Physics Communications, Vol. 183, Issue 3
A second nearest-neighbor embedded atom method interatomic potential for Li–Si alloys
journal, June 2012
- Cui, Zhiwei; Gao, Feng; Cui, Zhihua
- Journal of Power Sources, Vol. 207
Carbon enables the practical use of lithium metal in a battery
journal, October 2017
- Zhang, Chen; Huang, Zhijia; Lv, Wei
- Carbon, Vol. 123
Analysis of a Li-Ion Nanobattery with Graphite Anode Using Molecular Dynamics Simulations
journal, June 2017
- Ponce, Victor; Galvez-Aranda, Diego E.; Seminario, Jorge M.
- The Journal of Physical Chemistry C, Vol. 121, Issue 23
Implementing molecular dynamics on hybrid high performance computers – short range forces
journal, April 2011
- Brown, W. Michael; Wang, Peng; Plimpton, Steven J.
- Computer Physics Communications, Vol. 182, Issue 4
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions
journal, June 2002
- Aurbach, D.
- Solid State Ionics, Vol. 148, Issue 3-4
Reviving Lithium-Metal Anodes for Next-Generation High-Energy Batteries
journal, June 2017
- Guo, Yanpeng; Li, Huiqiao; Zhai, Tianyou
- Advanced Materials, Vol. 29, Issue 29
A computational investigation of thermal effect on lithium dendrite growth
journal, April 2018
- Yan, H. H.; Bie, Y. H.; Cui, X. Y.
- Energy Conversion and Management, Vol. 161
Nanostructured energy materials for electrochemical energy conversion and storage: A review
journal, November 2016
- Zhang, Xueqiang; Cheng, Xinbing; Zhang, Qiang
- Journal of Energy Chemistry, Vol. 25, Issue 6
Extensions of the molecular dynamics simulation method. II. Isothermal systems
journal, September 1983
- Haile, J. M.; Gupta, S.
- The Journal of Chemical Physics, Vol. 79, Issue 6
Certain Topics in Telegraph Transmission Theory
journal, April 1928
- Nyquist, H.
- Transactions of the American Institute of Electrical Engineers, Vol. 47, Issue 2
Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes
journal, January 2017
- Chen, Kuan-Hung; Wood, Kevin N.; Kazyak, Eric
- Journal of Materials Chemistry A, Vol. 5, Issue 23
Improved Graphite Anode for Lithium-Ion Batteries Chemically
journal, January 1996
- Peled, E.
- Journal of The Electrochemical Society, Vol. 143, Issue 1
Electrochemical intercalation of lithium into a natural graphite anode in quaternary ammonium-based ionic liquid electrolytes
journal, February 2006
- Zheng, Honghe; Jiang, Kai; Abe, Takeshi
- Carbon, Vol. 44, Issue 2
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool
journal, December 2009
- Stukowski, Alexander
- Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1
Perspectives for restraining harsh lithium dendrite growth: Towards robust lithium metal anodes
journal, November 2018
- Wu, Feng; Yuan, Yan-Xia; Cheng, Xin-Bing
- Energy Storage Materials, Vol. 15
Effect of the Electrolyte Composition on SEI Reactions at Si Anodes of Li-Ion Batteries
journal, March 2015
- Martinez de la Hoz, Julibeth M.; Soto, Fernando A.; Balbuena, Perla B.
- The Journal of Physical Chemistry C, Vol. 119, Issue 13
PACKMOL: A package for building initial configurations for molecular dynamics simulations
journal, October 2009
- Martínez, L.; Andrade, R.; Birgin, E. G.
- Journal of Computational Chemistry, Vol. 30, Issue 13
Reviving rechargeable lithium metal batteries: enabling next-generation high-energy and high-power cells
journal, January 2012
- Zhamu, Aruna; Chen, Guorong; Liu, Chenguang
- Energy Environ. Sci., Vol. 5, Issue 2
Interionic potentials in alkali halides and their use in simulations of the molten salts
journal, May 1976
- Sangster, M. J. L.; Dixon, M.
- Advances in Physics, Vol. 25, Issue 3
Critical review of the methods for monitoring of lithium-ion batteries in electric and hybrid vehicles
journal, July 2014
- Waag, Wladislaw; Fleischer, Christian; Sauer, Dirk Uwe
- Journal of Power Sources, Vol. 258
Molecular dynamics simulations of the first charge of a Li-ion—Si-anode nanobattery
journal, March 2017
- Galvez-Aranda, Diego E.; Ponce, Victor; Seminario, Jorge M.
- Journal of Molecular Modeling, Vol. 23, Issue 4
Modeling solid-electrolyte interfacial phenomena in silicon anodes
journal, August 2016
- Soto, Fa; Martinez de la Hoz, Jm; Seminario, Jm
- Current Opinion in Chemical Engineering, Vol. 13
The recent advances in constructing designed electrode in lithium metal batteries
journal, December 2017
- Cui, Jiecheng; Zhan, Tian-Guang; Zhang, Kang-Da
- Chinese Chemical Letters, Vol. 28, Issue 12, p. 2171-2179
The role of nanotechnology in the development of battery materials for electric vehicles
journal, December 2016
- Lu, Jun; Chen, Zonghai; Ma, Zifeng
- Nature Nanotechnology, Vol. 11, Issue 12
Simulations of a LiF Solid Electrolyte Interphase Cracking on Silicon Anodes Using Molecular Dynamics
journal, January 2018
- Galvez-Aranda, Diego E.; Seminario, Jorge M.
- Journal of The Electrochemical Society, Vol. 165, Issue 3
Crystallographic Data 186. Lithium
journal, December 1959
- Nadler, M. R/.; Kempier, C. P.
- Analytical Chemistry, Vol. 31, Issue 12
Lithium diffusion in silicon and induced structure disorder: A molecular dynamics study
journal, November 2013
- Wang, Huanyu; Ji, Xiao; Chen, Chi
- AIP Advances, Vol. 3, Issue 11
VMD: Visual molecular dynamics
journal, February 1996
- Humphrey, William; Dalke, Andrew; Schulten, Klaus
- Journal of Molecular Graphics, Vol. 14, Issue 1
Lithium-Ion Model Behavior in an Ethylene Carbonate Electrolyte Using Molecular Dynamics
journal, July 2016
- Kumar, Narendra; Seminario, Jorge M.
- The Journal of Physical Chemistry C, Vol. 120, Issue 30
Works referencing / citing this record:
Enhancement of the electrochemical performance of lithium-ion batteries by SiO 2 @poly(2-acrylamido-2-methylpropanesulfonic acid) nanosphere addition into a polypropylene membrane
journal, January 2020
- Yang, Guoping; Cai, Haopeng; Li, Xiangyu
- RSC Advances, Vol. 10, Issue 9