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Title: Dendrite formation in silicon anodes of lithium-ion batteries

Abstract

Rechargeable lithium-ion batteries require a vigorous improvement if we want to use them massively for high energy applications. Silicon and metal lithium anodes are excellent alternatives because of their large theoretical capacity when compared to graphite used in practically all rechargeable Li-ion batteries. However, several problems need to be addressed satisfactorily before a major fabrication effort can be launched; for instance, the growth of lithium dendrites is one of the most important to take care due to safety issues. In this work we attempt to predict the mechanism of dendrite growth by simulating possible behaviors of charge distributions in the anode of an already cracked solid electrolyte interphase of a nanobattery, which is under the application of an external field representing the charging of the battery; thus, elucidating the conditions for dendrite growth. The extremely slow drift velocity of the Li-ions of ~1 mm per hour in a typical commercial Li-ion battery, makes the growth of a dendrite take a few hours; however, once a Li-ion arrives at an active site of the anode, it takes an extremely short time of ~1 ps to react. This large difference in time-scales allows us to perform the molecular dynamics simulation of themore » ions at much larger drift velocities, so we can have valuable results in reasonable computational times. The conditions before the growth are assumed and conditions that do not lead to the growth are ignored. We performed molecular dynamics simulations of a pre-lithiated silicon anode with a Li : Si ratio of 21 : 5, corresponding to a fully charged battery. We simulate the dendrite growth by testing a few charge distributions in a nanosized square representing a crack of the solid electrolyte interphase, which is where the electrolyte solution comes into direct contact with the LiSi alloy anode. Depending on the selected charge distributions for such an anode surface, the dendrites grow during the simulation when an external field is applied. We found that dendrites grow when strong deviations of charge distributions take place on the surface of the crack. Results from this work are important in finding ways to constrain lithium dendrite growth using tailored coatings or pre-coatings covering the LiSi alloy anode.« less

Authors:
 [1]; ORCiD logo [1]
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  1. 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)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1418385
Alternate Identifier(s):
OSTI ID: 1545320
Grant/Contract Number:  
EE0007766
Resource Type:
Published Article
Journal Name:
RSC Advances
Additional Journal Information:
Journal Name: RSC Advances Journal Volume: 8 Journal Issue: 10; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Selis, Luis A., and Seminario, Jorge M. Dendrite formation in silicon anodes of lithium-ion batteries. United Kingdom: N. p., 2018. Web. doi:10.1039/C7RA12690E.
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Selis, Luis A., & Seminario, Jorge M. Dendrite formation in silicon anodes of lithium-ion batteries. United Kingdom. https://doi.org/10.1039/C7RA12690E
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Selis, Luis A., and Seminario, Jorge M. Mon . "Dendrite formation in silicon anodes of lithium-ion batteries". United Kingdom. https://doi.org/10.1039/C7RA12690E.
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@article{osti_1418385,
title = {Dendrite formation in silicon anodes of lithium-ion batteries},
author = {Selis, Luis A. and Seminario, Jorge M.},
abstractNote = {Rechargeable lithium-ion batteries require a vigorous improvement if we want to use them massively for high energy applications. Silicon and metal lithium anodes are excellent alternatives because of their large theoretical capacity when compared to graphite used in practically all rechargeable Li-ion batteries. However, several problems need to be addressed satisfactorily before a major fabrication effort can be launched; for instance, the growth of lithium dendrites is one of the most important to take care due to safety issues. In this work we attempt to predict the mechanism of dendrite growth by simulating possible behaviors of charge distributions in the anode of an already cracked solid electrolyte interphase of a nanobattery, which is under the application of an external field representing the charging of the battery; thus, elucidating the conditions for dendrite growth. The extremely slow drift velocity of the Li-ions of ~1 mm per hour in a typical commercial Li-ion battery, makes the growth of a dendrite take a few hours; however, once a Li-ion arrives at an active site of the anode, it takes an extremely short time of ~1 ps to react. This large difference in time-scales allows us to perform the molecular dynamics simulation of the ions at much larger drift velocities, so we can have valuable results in reasonable computational times. The conditions before the growth are assumed and conditions that do not lead to the growth are ignored. We performed molecular dynamics simulations of a pre-lithiated silicon anode with a Li : Si ratio of 21 : 5, corresponding to a fully charged battery. We simulate the dendrite growth by testing a few charge distributions in a nanosized square representing a crack of the solid electrolyte interphase, which is where the electrolyte solution comes into direct contact with the LiSi alloy anode. Depending on the selected charge distributions for such an anode surface, the dendrites grow during the simulation when an external field is applied. We found that dendrites grow when strong deviations of charge distributions take place on the surface of the crack. Results from this work are important in finding ways to constrain lithium dendrite growth using tailored coatings or pre-coatings covering the LiSi alloy anode.},
doi = {10.1039/C7RA12690E},
journal = {RSC Advances},
number = 10,
volume = 8,
place = {United Kingdom},
year = {2018},
month = {1}
}
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Works referenced in this record:

Universal equation of state
journal, July 1988

A strategy of selective and dendrite-free lithium deposition for lithium batteries
journal, December 2017

Suppression of lithium dendrite growth by introducing a low reduction potential complex cation in the electrolyte
journal, January 2016

Electron transfer through solid-electrolyte-interphase layers formed on Si anodes of Li-ion batteries
journal, September 2014

Electrolyte additive enabled fast charging and stable cycling lithium metal batteries
journal, March 2017

The Dielectric Constants of Ethylene Carbonate and of Solutions of Ethylene Carbonate in Water, Methanol, Benzene and Propylene Carbonate
journal, January 1958

  • Seward, Ralph P.; Vieira, Ernest C.
  • The Journal of Physical Chemistry, Vol. 62, Issue 1
  • DOI: 10.1021/j150559a041

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
  • DOI: 10.1021/ja00051a040

Porous Si anode materials for lithium rechargeable batteries
journal, January 2010

  • Cho, Jaephil
  • Journal of Materials Chemistry, Vol. 20, Issue 20
  • DOI: 10.1039/b923002e

Modified embedded-atom method interatomic potentials for the Ni–Co binary and the Ni–Al–Co ternary systems
journal, May 2015

  • Kim, Young-Kwang; Jung, Woo-Sang; Lee, Byeong-Joo
  • Modelling and Simulation in Materials Science and Engineering, Vol. 23, Issue 5
  • DOI: 10.1088/0965-0393/23/5/055004

Lithium dendrite growth mechanisms in liquid electrolytes
journal, November 2017

Structures, phase stabilities, and electrical potentials of Li-Si battery anode materials
journal, May 2013

Geometric and electronic studies of Li15Si4 for silicon anode
journal, December 2008

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Accurate Standard Hydrogen Electrode Potential and Applications to the Redox Potentials of Vitamin C and NAD/NADH
journal, January 2015

  • Matsui, Toru; Kitagawa, Yasutaka; Okumura, Mitsutaka
  • The Journal of Physical Chemistry A, Vol. 119, Issue 2
  • DOI: 10.1021/jp508308y

Review of gel-type polymer electrolytes for lithium-ion batteries
journal, February 1999

Promises and challenges of nanomaterials for lithium-based rechargeable batteries
journal, June 2016

Atomistic Modeling of the Electrode–Electrolyte Interface in Li-Ion Energy Storage Systems: Electrolyte Structuring
journal, February 2013

  • Jorn, Ryan; Kumar, Revati; Abraham, Daniel P.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 8
  • DOI: 10.1021/jp3102282

Structure and Properties of Li−Si Alloys: A First-Principles Study
journal, December 2010

  • Kim, Hyunwoo; Chou, Chia-Yun; Ekerdt, John G.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 5
  • DOI: 10.1021/jp1083899

Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
journal, October 2004

Annealing kinetics of electrodeposited lithium dendrites
journal, October 2015

  • Aryanfar, Asghar; Cheng, Tao; Colussi, Agustin J.
  • The Journal of Chemical Physics, Vol. 143, Issue 13
  • DOI: 10.1063/1.4930014

Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study
journal, December 2016

  • Barai, Pallab; Higa, Kenneth; Srinivasan, Venkat
  • Journal of The Electrochemical Society, Vol. 164, Issue 2
  • DOI: 10.1149/2.0661702jes

Lithium metal anodes for rechargeable batteries
journal, January 2014

  • Xu, Wu; Wang, Jiulin; Ding, Fei
  • Energy Environ. Sci., Vol. 7, Issue 2
  • DOI: 10.1039/C3EE40795K

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
  • DOI: 10.1039/C6EE01674J

Dendrite-Suppressed Lithium Plating from a Liquid Electrolyte via Wetting of Li 3 N
journal, July 2017

Lithium Alloying Potentials of Silicon as Anode of Lithium Secondary Batteries
journal, January 2013

A review on the key issues for lithium-ion battery management in electric vehicles
journal, March 2013

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
  • DOI: 10.1038/nnano.2014.152

FIRST IMAGES OF NANOBUBBLES: Study proves existence of tiny air bubbles on colloid surfaces
journal, October 2001

Ethylene Carbonate−Li + :  A Theoretical Study of Structural and Vibrational Properties in Gas and Liquid Phases
journal, February 2004

  • Masia, Marco; Probst, Michael; Rey, Rossend
  • The Journal of Physical Chemistry B, Vol. 108, Issue 6
  • DOI: 10.1021/jp036673w

Lithium fluoride dissolution equilibria in cyclic alkylcarbonates and water
journal, May 2010

  • Jones, Jennifer; Anouti, Mérièm; Caillon-Caravanier, Magaly
  • Journal of Molecular Liquids, Vol. 153, Issue 2-3
  • DOI: 10.1016/j.molliq.2010.02.006

Characterization of commercially available lithium-ion batteries
journal, January 1998

A second nearest-neighbor embedded atom method interatomic potential for Li–Si alloys
journal, June 2012

Polyhedral approximation and practical convex hull algorithm for certain classes of voxel sets
journal, August 2009

Nanoporous Polymer-Ceramic Composite Electrolytes for Lithium Metal Batteries
journal, September 2013

  • Tu, Zhengyuan; Kambe, Yu; Lu, Yingying
  • Advanced Energy Materials, Vol. 4, Issue 2, Article No. 1300654
  • DOI: 10.1002/aenm.201300654

Electron Transport and Electrolyte Reduction in the Solid-Electrolyte Interphase of Rechargeable Lithium Ion Batteries with Silicon Anodes
journal, August 2016

  • Benitez, Laura; Seminario, Jorge M.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 32
  • DOI: 10.1021/acs.jpcc.6b06446

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
  • DOI: 10.1021/acs.jpcc.7b04190

Surface effects on the structure and lithium behavior in lithiated silicon: A first principles study
journal, June 2013

Suppression of Dendrite Formation by Using a Hydrogel Separator for Zinc Alkaline Battery
journal, January 2017

Universal features of the equation of state of metals
journal, March 1984

An ab Initio CFF93 All-Atom Force Field for Polycarbonates
journal, April 1994

  • Sun, Huai; Mumby, Stephen J.; Maple, Jon R.
  • Journal of the American Chemical Society, Vol. 116, Issue 7
  • DOI: 10.1021/ja00086a030

Packing optimization for automated generation of complex system's initial configurations for molecular dynamics and docking
journal, May 2003

  • Martínez, José Mario; Martínez, Leandro
  • Journal of Computational Chemistry, Vol. 24, Issue 7
  • DOI: 10.1002/jcc.10216

ReaxFF:  A Reactive Force Field for Hydrocarbons
journal, October 2001

  • van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois
  • The Journal of Physical Chemistry A, Vol. 105, Issue 41
  • DOI: 10.1021/jp004368u

First principles studies of silicon as a negative electrode material for lithium-ion batteries
journal, June 2009

  • Chevrier, V. L.; Zwanziger, J. W.; Dahn, J. R.
  • Canadian Journal of Physics, Vol. 87, Issue 6
  • DOI: 10.1139/P09-031

Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool
journal, December 2009

Designing nanostructured Si anodes for high energy lithium ion batteries
journal, October 2012

Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism
journal, March 2013

  • Ding, Fei; Xu, Wu; Graff, Gordon L.
  • Journal of the American Chemical Society, Vol. 135, Issue 11, p. 4450-4456
  • DOI: 10.1021/ja312241y

State of the art of commercial Li ion batteries
journal, December 2000

Selective deposition and stable encapsulation of lithium through heterogeneous seeded growth
journal, February 2016

  • Yan, Kai; Lu, Zhenda; Lee, Hyun-Wook
  • Nature Energy, Vol. 1, Issue 3, Article No. 16010
  • DOI: 10.1038/nenergy.2016.10

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
  • DOI: 10.1002/jcc.21224

Fluoroethylene Carbonate Additives to Render Uniform Li Deposits in Lithium Metal Batteries
journal, January 2017

  • Zhang, Xue-Qiang; Cheng, Xin-Bing; Chen, Xiang
  • Advanced Functional Materials, Vol. 27, Issue 10
  • DOI: 10.1002/adfm.201605989

Garnet-type solid-state fast Li ion conductors for Li batteries: critical review
journal, January 2014

  • Thangadurai, Venkataraman; Narayanan, Sumaletha; Pinzaru, Dana
  • Chemical Society Reviews, Vol. 43, Issue 13
  • DOI: 10.1039/c4cs00020j

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
  • DOI: 10.1007/s00894-017-3283-2

Molecular Spectra and Molecular Structure
book, January 1979

Suppressing Lithium Dendrite Growth by Metallic Coating on a Separator
journal, October 2017

  • Lee, Hongkyung; Ren, Xiaodi; Niu, Chaojiang
  • Advanced Functional Materials, Vol. 27, Issue 45
  • DOI: 10.1002/adfm.201704391

Direct in situ observation and explanation of lithium dendrite of commercial graphite electrodes
journal, January 2015

  • Guo, Zhansheng; Zhu, Jianyu; Feng, Jiemin
  • RSC Advances, Vol. 5, Issue 85
  • DOI: 10.1039/C5RA13289D

History, Evolution, and Future Status of Energy Storage
journal, May 2012

Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

Dendrite Growth in Lithium/Polymer Systems
journal, January 2003

  • Monroe, Charles; Newman, John
  • Journal of The Electrochemical Society, Vol. 150, Issue 10
  • DOI: 10.1149/1.1606686

Crystallographic Data 186. Lithium
journal, December 1959

  • Nadler, M. R/.; Kempier, C. P.
  • Analytical Chemistry, Vol. 31, Issue 12
  • DOI: 10.1021/ac60156a007

Ab initio study of the electronic structures of lithium containing diatomic molecules and ions
journal, December 1993

  • Boldyrev, Alexander I.; Simons, Jack; Schleyer, Paul von R.
  • The Journal of Chemical Physics, Vol. 99, Issue 11
  • DOI: 10.1063/1.465600

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
  • DOI: 10.1063/1.4829440

VMD: Visual molecular dynamics
journal, February 1996

A Review of Solid Electrolyte Interphases on Lithium Metal Anode
journal, November 2015

Stable lithium electrodeposition in liquid and nanoporous solid electrolytes
journal, August 2014

  • Lu, Yingying; Tu, Zhengyuan; Archer, Lynden A.
  • Nature Materials, Vol. 13, Issue 10
  • DOI: 10.1038/nmat4041

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
  • DOI: 10.1021/acs.jpcc.6b03709

Dielectric Relaxation of Ethylene Carbonate and Propylene Carbonate from Molecular Dynamics Simulations
journal, November 2015

  • You, Xinli; Chaudhari, Mangesh I.; Rempe, Susan B.
  • The Journal of Physical Chemistry B, Vol. 120, Issue 8
  • DOI: 10.1021/acs.jpcb.5b09561
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