Molecular dynamics simulations of the first charge of a Li-ion—Si-anode nanobattery

Galvez-Aranda, Diego E.; Ponce, Victor; Seminario, Jorge M.

doi:10.1007/s00894-017-3283-2

Title: Molecular dynamics simulations of the first charge of a Li-ion—Si-anode nanobattery

Journal Article · Thu Mar 16 00:00:00 EDT 2017 · Journal of Molecular Modeling

DOI:https://doi.org/10.1007/s00894-017-3283-2· OSTI ID:1430651

Galvez-Aranda, Diego E. ^[1]; Ponce, Victor ^[1];

^[2]

Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering, Department of Electrical and Computer Engineering and Department of Materials Science and Engineering

Rechargeable lithium-ion batteries are the most popular devices for energy storage but still a lot of research needs to be done to improve their cycling and storage capacity. Silicon has been proposed as an anode material because of its large theoretical capacity of ~3600 mAh/g. Therefore, focus is needed on the lithiation process of silicon anodes where it is known that the anode increases its volume more than 300%, producing cracking and other damages. In this study, we performed molecular dynamics atomistic simulations to study the swelling, alloying, and amorphization of a silicon nanocrystal anode in a full nanobattery model during the first charging cycle. A dissolved salt of lithium hexafluorophosphate in ethylene carbonate was chosen as the electrolyte solution and lithium cobalt oxide as cathode. External electric fields are applied to emulate the charging, causing the migration of the Li-ions from the cathode to the anode, by drifting through the electrolyte solution, thus converting pristine Si gradually into Li₁₄Si₅ when fully lithiated. When the electric field is applied to the nanobattery, the temperature never exceeds 360 K due to a temperature control imposed resembling a cooling mechanism. The volume of the anode increases with the amorphization of the silicon as the external field is applied by creating a layer of LiSi alloy between the electrolyte and the silicon nanocrystal and then, at the arrival of more Li-ions changing to an alloy, where the drift velocity of Li-ions is greater than the velocity in the initial nanocrystal structure. Charge neutrality is maintained by concerted complementary reduction-oxidation reactions at the anode and cathode, respectively. Also, the nanobattery model developed here can be used to study charge mobility, current density, conductance and resistivity, among several other properties of several candidate materials for rechargeable batteries and constitutes the initial point for further studies on the formation of the solid electrolyte interphase in the anode.

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Research Organization:: 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), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: EE0007766; AC02-05CH11231

OSTI ID:: 1430651

Journal Information:: Journal of Molecular Modeling, Vol. 23, Issue 4; ISSN 1610-2940

Publisher:: Springer-VerlagCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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References (55)

Ab Initio Analysis of Silicon Nano-Clusters Aguilera-Segura, Sonia M.; Seminario, Jorge M. The Journal of Physical Chemistry C, Vol. 118, Issue 2 https://doi.org/10.1021/jp410975s	journal	December 2013
Universal equation of state Jeanloz, Raymond Physical Review B, Vol. 38, Issue 1 https://doi.org/10.1103/PhysRevB.38.805	journal	July 1988
Challenges for Rechargeable Li Batteries Goodenough, John B.; Kim, Youngsik Chemistry of Materials, Vol. 22, Issue 3, p. 587-603 https://doi.org/10.1021/cm901452z	journal	February 2010
Electronic Population Analysis on LCAO‐MO Molecular Wave Functions. III. Effects of Hybridization on Overlap and Gross AO Populations Mulliken, R. S. The Journal of Chemical Physics, Vol. 23, Issue 12 https://doi.org/10.1063/1.1741876	journal	December 1955
Electron transfer through solid-electrolyte-interphase layers formed on Si anodes of Li-ion batteries Benitez, L.; Cristancho, D.; Seminario, J. M. Electrochimica Acta, Vol. 140 https://doi.org/10.1016/j.electacta.2014.05.018	journal	September 2014
Electronic Population Analysis on LCAO‐MO Molecular Wave Functions. IV. Bonding and Antibonding in LCAO and Valence‐Bond Theories Mulliken, R. S. The Journal of Chemical Physics, Vol. 23, Issue 12 https://doi.org/10.1063/1.1741877	journal	December 1955
UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations Rappe, A. K.; Casewit, C. J.; Colwell, K. S. Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035 https://doi.org/10.1021/ja00051a040	journal	December 1992
Charge–discharge stability of graphite anodes for lithium-ion batteries Wang, Chunsheng; Appleby, A. John; Little, Frank E. Journal of Electroanalytical Chemistry, Vol. 497, Issue 1-2 https://doi.org/10.1016/S0022-0728(00)00447-2	journal	February 2001
Modified embedded-atom method interatomic potentials for the Ni–Co binary and the Ni–Al–Co ternary systems Kim, Young-Kwang; Jung, Woo-Sang; Lee, Byeong-Joo Modelling and Simulation in Materials Science and Engineering, Vol. 23, Issue 5 https://doi.org/10.1088/0965-0393/23/5/055004	journal	May 2015
Volume Expansion during Lithiation of Amorphous Silicon Thin Film Electrodes Studied by In-Operando Neutron Reflectometry Jerliu, B.; Hüger, E.; Dörrer, L. The Journal of Physical Chemistry C, Vol. 118, Issue 18 https://doi.org/10.1021/jp502261t	journal	April 2014
High-performance lithium battery anodes using silicon nanowires Chan, Candace K.; Peng, Hailin; Liu, Gao Nature Nanotechnology, Vol. 3, Issue 1, p. 31-35 https://doi.org/10.1038/nnano.2007.411	journal	December 2007
In situ atomic-scale imaging of electrochemical lithiation in silicon Liu, Xiao Hua; Wang, Jiang Wei; Huang, Shan Nature Nanotechnology, Vol. 7, Issue 11 https://doi.org/10.1038/nnano.2012.170	journal	October 2012
First principles study of lithium insertion in bulk silicon Wan, Wenhui; Zhang, Qianfan; Cui, Yi Journal of Physics: Condensed Matter, Vol. 22, Issue 41 https://doi.org/10.1088/0953-8984/22/41/415501	journal	September 2010
Gaston Planté and his invention of the lead–acid battery—The genesis of the first practical rechargeable battery Kurzweil, P. Journal of Power Sources, Vol. 195, Issue 14 https://doi.org/10.1016/j.jpowsour.2009.12.126	journal	July 2010
Geometric and electronic studies of Li15Si4 for silicon anode Xu, Yu Hong; Yin, Ge Ping; Zuo, Peng Jian Electrochimica Acta, Vol. 54, Issue 2 https://doi.org/10.1016/j.electacta.2008.07.083	journal	December 2008
Spectroscopic properties of 41 electronic states of Pd ₂ Balasubramanian, K. The Journal of Chemical Physics, Vol. 89, Issue 10 https://doi.org/10.1063/1.455397	journal	November 1988
Review of gel-type polymer electrolytes for lithium-ion batteries Song, J. Y.; Wang, Y. Y.; Wan, C. C. Journal of Power Sources, Vol. 77, Issue 2, p. 183-197 https://doi.org/10.1016/S0378-7753(98)00193-1	journal	February 1999
Structure and Reactivity of Alucone-Coated Films on Si and Li _x Si _y Surfaces Ma, Yuguang; Martinez de la Hoz, Julibeth M.; Angarita, Ivette ACS Applied Materials & Interfaces, Vol. 7, Issue 22 https://doi.org/10.1021/acsami.5b01917	journal	May 2015
Comparative Issues of Cathode Materials for Li-Ion Batteries Julien, Christian; Mauger, Alain; Zaghib, Karim Inorganics, Vol. 2, Issue 1 https://doi.org/10.3390/inorganics2010132	journal	March 2014
Lithium metal anodes for rechargeable batteries Xu, Wu; Wang, Jiulin; Ding, Fei Energy Environ. Sci., Vol. 7, Issue 2 https://doi.org/10.1039/C3EE40795K	journal	January 2014
In Situ XRD and Electrochemical Study of the Reaction of Lithium with Amorphous Silicon Hatchard, T. D.; Dahn, J. R. Journal of The Electrochemical Society, Vol. 151, Issue 6 https://doi.org/10.1149/1.1739217	journal	January 2004
Stable cycling of double-walled silicon nanotube battery anodes through solid–electrolyte interphase control Wu, Hui; Chan, Gerentt; Choi, Jang Wook Nature Nanotechnology, Vol. 7, Issue 5 https://doi.org/10.1038/nnano.2012.35	journal	March 2012
Electronic Population Analysis on LCAO–MO Molecular Wave Functions. II. Overlap Populations, Bond Orders, and Covalent Bond Energies Mulliken, R. S. The Journal of Chemical Physics, Vol. 23, Issue 10 https://doi.org/10.1063/1.1740589	journal	October 1955
A review on the key issues for lithium-ion battery management in electric vehicles Lu, Languang; Han, Xuebing; Li, Jianqiu Journal of Power Sources, Vol. 226, p. 272-288 https://doi.org/10.1016/j.jpowsour.2012.10.060	journal	March 2013
Computational Studies of Interfacial Reactions at Anode Materials: Initial Stages of the Solid-Electrolyte-Interphase Layer Formation Ramos-Sanchez, G.; Soto, F. A.; Martinez de la Hoz, J. M. Journal of Electrochemical Energy Conversion and Storage, Vol. 13, Issue 3 https://doi.org/10.1115/1.4034412	journal	August 2016
Electronic Population Analysis on LCAO–MO Molecular Wave Functions. I Mulliken, R. S. The Journal of Chemical Physics, Vol. 23, Issue 10 https://doi.org/10.1063/1.1740588	journal	October 1955
Molecular dynamics simulations at constant pressure and/or temperature Andersen, Hans C. The Journal of Chemical Physics, Vol. 72, Issue 4 https://doi.org/10.1063/1.439486	journal	February 1980
Li diffusion in LiCoO2 thin films prepared by pulsed laser deposition Xia, Hui; Lu, Li; Ceder, G. Journal of Power Sources, Vol. 159, Issue 2 https://doi.org/10.1016/j.jpowsour.2005.12.012	journal	September 2006
Thermal-runaway experiments on consumer Li-ion batteries with metal-oxide and olivin-type cathodes Golubkov, Andrey W.; Fuchs, David; Wagner, Julian RSC Adv., Vol. 4, Issue 7 https://doi.org/10.1039/C3RA45748F	journal	January 2014
Silicon Nanowire Fabric as a Lithium Ion Battery Electrode Material Chockla, Aaron M.; Harris, Justin T.; Akhavan, Vahid A. Journal of the American Chemical Society, Vol. 133, Issue 51 https://doi.org/10.1021/ja208232h	journal	December 2011
Lithium fluoride dissolution equilibria in cyclic alkylcarbonates and water Jones, Jennifer; Anouti, Mérièm; Caillon-Caravanier, Magaly Journal of Molecular Liquids, Vol. 153, Issue 2-3 https://doi.org/10.1016/j.molliq.2010.02.006	journal	May 2010
Two-Phase Electrochemical Lithiation in Amorphous Silicon Wang, Jiang Wei; He, Yu; Fan, Feifei Nano Letters, Vol. 13, Issue 2 https://doi.org/10.1021/nl304379k	journal	January 2013
Formation and Growth Mechanisms of Solid-Electrolyte Interphase Layers in Rechargeable Batteries Soto, Fernando A.; Ma, Yuguang; Martinez de la Hoz, Julibeth M. Chemistry of Materials, Vol. 27, Issue 23 https://doi.org/10.1021/acs.chemmater.5b03358	journal	November 2015
A second nearest-neighbor embedded atom method interatomic potential for Li–Si alloys Cui, Zhiwei; Gao, Feng; Cui, Zhihua Journal of Power Sources, Vol. 207 https://doi.org/10.1016/j.jpowsour.2012.01.145	journal	June 2012
Polyhedral approximation and practical convex hull algorithm for certain classes of voxel sets Schulz, Henrik Discrete Applied Mathematics, Vol. 157, Issue 16 https://doi.org/10.1016/j.dam.2009.04.008	journal	August 2009
Electron Transport and Electrolyte Reduction in the Solid-Electrolyte Interphase of Rechargeable Lithium Ion Batteries with Silicon Anodes Benitez, Laura; Seminario, Jorge M. The Journal of Physical Chemistry C, Vol. 120, Issue 32 https://doi.org/10.1021/acs.jpcc.6b06446	journal	August 2016
Recent developments in lithium ion batteries Wakihara, Masataka Materials Science and Engineering: R: Reports, Vol. 33, Issue 4 https://doi.org/10.1016/S0927-796X(01)00030-4	journal	June 2001
All-Solid Lithium Electrodes with Mixed-Conductor Matrix Boukamp, B. A. Journal of The Electrochemical Society, Vol. 128, Issue 4 https://doi.org/10.1149/1.2127495	journal	January 1981
In Situ TEM of Two-Phase Lithiation of Amorphous Silicon Nanospheres McDowell, Matthew T.; Lee, Seok Woo; Harris, Justin T. Nano Letters, Vol. 13, Issue 2 https://doi.org/10.1021/nl3044508	journal	January 2013
Universal features of the equation of state of metals Rose, James H.; Smith, John R.; Guinea, Francisco Physical Review B, Vol. 29, Issue 6 https://doi.org/10.1103/PhysRevB.29.2963	journal	March 1984
Electrochemical behaviors of silicon based anode material Yoshio, Masaki; Kugino, Satoshi; Dimov, Nikolay Journal of Power Sources, Vol. 153, Issue 2 https://doi.org/10.1016/j.jpowsour.2005.05.052	journal	February 2006
Investigation of Lithium Insertion Mechanisms of a Thin-Film Si Electrode by Coupling Time-of-Flight Secondary-Ion Mass Spectrometry, X-ray Photoelectron Spectroscopy, and Focused-Ion-Beam/SEM Bordes, Arnaud; De Vito, Eric; Haon, Cédric ACS Applied Materials & Interfaces, Vol. 7, Issue 50 https://doi.org/10.1021/acsami.5b09261	journal	December 2015
Vacancies in Si Can Improve the Concentration-Dependent Lithiation Rate: Molecular Dynamics Studies of Lithiation Dynamics of Si Electrodes Kim, Kwang Jin; Qi, Yue The Journal of Physical Chemistry C, Vol. 119, Issue 43 https://doi.org/10.1021/acs.jpcc.5b06953	journal	October 2015
Diffusion Rate of Li in Si at Low Temperatures Pell, E. M. Physical Review, Vol. 119, Issue 4 https://doi.org/10.1103/PhysRev.119.1222	journal	August 1960
A theoretical study of lithium absorption in amorphous and crystalline silicon Popov, Z. I.; Fedorov, A. S.; Kuzubov, A. A. Journal of Structural Chemistry, Vol. 52, Issue 5 https://doi.org/10.1134/s0022476611050039	journal	October 2011
Determination of the diffusion coefficient of lithium ions in nano-Si Ding, N.; Xu, J.; Yao, Y. X. Solid State Ionics, Vol. 180, Issue 2-3 https://doi.org/10.1016/j.ssi.2008.12.015	journal	March 2009
Ab initio study of the electronic structures of lithium containing diatomic molecules and ions Boldyrev, Alexander I.; Simons, Jack; Schleyer, Paul von R. The Journal of Chemical Physics, Vol. 99, Issue 11 https://doi.org/10.1063/1.465600	journal	December 1993
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction Obrovac, M. N.; Christensen, Leif Electrochemical and Solid-State Letters, Vol. 7, Issue 5 https://doi.org/10.1149/1.1652421	journal	January 2004
Lithium diffusion in silicon and induced structure disorder: A molecular dynamics study Wang, Huanyu; Ji, Xiao; Chen, Chi AIP Advances, Vol. 3, Issue 11 https://doi.org/10.1063/1.4829440	journal	November 2013
Lithium-Ion Model Behavior in an Ethylene Carbonate Electrolyte Using Molecular Dynamics Kumar, Narendra; Seminario, Jorge M. The Journal of Physical Chemistry C, Vol. 120, Issue 30 https://doi.org/10.1021/acs.jpcc.6b03709	journal	July 2016
In situ TEM electrochemistry of anode materials in lithium ion batteries Liu, Xiao Hua; Huang, Jian Yu Energy & Environmental Science, Vol. 4, Issue 10 https://doi.org/10.1039/c1ee01918j	journal	January 2011
Study of lithiation mechanisms in silicon electrodes by Auger Electron Spectroscopy Radvanyi, Etienne; De Vito, Eric; Porcher, Willy Journal of Materials Chemistry A, Vol. 1, Issue 16 https://doi.org/10.1039/c3ta10212b	journal	January 2013
Adaptive State-of-Charge Indication System for Li-ion Battery-Powered Devices Pop, V.; Bergveld, H. J.; Danilov, D. World Electric Vehicle Journal, Vol. 1, Issue 1 https://doi.org/10.3390/wevj1010038	journal	December 2007
High-performance lithium battery anodes using silicon nanowires Chan, Candace K.; Peng, Hailin; Liu, Gao Materials for Sustainable Energy: A Collection of Peer-Reviewed Research and Review Articles from Nature Publishing Group, p. 187-191 https://doi.org/10.1142/9789814317665_0026	book	October 2010
Electrochemical behaviors of silicon based anode material Yoshio, Masaki; Tsumura, Takaaki; Dimov, Nikolay Journal of Power Sources, Vol. 146, Issue 1-2, p. 10-14 https://doi.org/10.1016/j.jpowsour.2005.03.143	journal	August 2005

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Title: Molecular dynamics simulations of the first charge of a Li-ion—Si-anode nanobattery

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