Accurate Calculation of Solvation Properties of Lithium Ions in Nonaqueous Solutions

Vigil, Daniel L.; Stevens, Mark J.; Frischknecht, Amalie L.

doi:10.1021/acs.jpcb.3c05591

Title: Accurate Calculation of Solvation Properties of Lithium Ions in Nonaqueous Solutions

Journal Article · 07 September 2023 · Journal of Physical Chemistry. B

DOI: https://doi.org/10.1021/acs.jpcb.3c05591 · OSTI ID:2311353

^[1];

^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Here, we perform all-atom molecular dynamics simulations of lithium triflate in 1,2-dimethoxyethane using six different literature force fields. This system is representative of many experimental studies of lithium salts in solvents and polymers. We show that multiple historically common force fields for lithium ions give qualitatively incorrect results when compared with those from experiments and quantum chemistry calculations. We illustrate the importance of correctly selecting force field parameters and give recommendations on the force field choice for lithium electrolyte applications.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: NA0003525

OSTI ID:: 2311353

Report Number(s):: SAND-2023-10791J

Journal Information:: Journal of Physical Chemistry. B, Vol. 127, Issue 37; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (69)

The Hydration Number of Li ⁺ in Liquid Water Rempe, Susan B.; Pratt, Lawrence R.; Hummer, Gerhard Journal of the American Chemical Society, Vol. 122, Issue 5 https://doi.org/10.1021/ja9924750	journal	February 2000
Spectroscopic studies of ionic solvation. XVIII. Solvation of the lithium ion in acetone and acetone-nitromethane mixtures Baum, Robert G.; Popov, Alexander I. Journal of Solution Chemistry, Vol. 4, Issue 5 https://doi.org/10.1007/BF00645576	journal	May 1975
Structures of [Li(glyme)] ⁺ complexes and their interactions with anions in equimolar mixtures of glymes and Li[TFSA]: analysis by molecular dynamics simulations Tsuzuki, Seiji; Shinoda, Wataru; Matsugami, Masaru Physical Chemistry Chemical Physics, Vol. 17, Issue 1 https://doi.org/10.1039/C4CP04718D	journal	January 2015
Development of nonadditive intermolecular potentials using molecular dynamics: Solvation of Li ⁺ and F ⁻ ions in polarizable water Dang, Liem X. The Journal of Chemical Physics, Vol. 96, Issue 9 https://doi.org/10.1063/1.462555	journal	May 1992
Accounting for electronic polarization in non-polarizable force fields Leontyev, Igor; Stuchebrukhov, Alexei Physical Chemistry Chemical Physics, Vol. 13, Issue 7 https://doi.org/10.1039/c0cp01971b	journal	January 2011
Temperature-Dependent Elasticity of a Semicrystalline Interphase Composed of Freely Rotating Chains in 't Veld, Pieter J.; Rutledge, Gregory C. Macromolecules, Vol. 36, Issue 19 https://doi.org/10.1021/ma0346658	journal	September 2003
Solvate ionic liquids based on lithium bis(trifluoromethanesulfonyl)imide–glyme systems: coordination in MD simulations with scaled charges Thum, Andreas; Heuer, Andreas; Shimizu, Karina Physical Chemistry Chemical Physics, Vol. 22, Issue 2 https://doi.org/10.1039/C9CP04947A	journal	January 2020
A Raman study of ion—polymer and ion—ion interactions in low molecular weight polyether—LiCF3SO3 complexes Petersen, G.; Jacobsson, P.; Torell, L. M. Electrochimica Acta, Vol. 37, Issue 9 https://doi.org/10.1016/0013-4686(92)80097-6	journal	January 1992
Modeling electrode polarization in dielectric spectroscopy: Ion mobility and mobile ion concentration of single-ion polymer electrolytes Klein, Robert J.; Zhang, Shihai; Dou, Shichen The Journal of Chemical Physics, Vol. 124, Issue 14 https://doi.org/10.1063/1.2186638	journal	April 2006
Role of Mixed Solvation and Ion Pairing in the Solution Structure of Lithium Ion Battery Electrolytes Seo, Daniel M.; Reininger, Stefanie; Kutcher, Mary The Journal of Physical Chemistry C, Vol. 119, Issue 25 https://doi.org/10.1021/acs.jpcc.5b03694	journal	June 2015
Effects of Ion Atmosphere on Hydrogen-Bond Dynamics in Aqueous Electrolyte Solutions Chandra, Amalendu Physical Review Letters, Vol. 85, Issue 4 https://doi.org/10.1103/PhysRevLett.85.768	journal	July 2000
Application of Static Charge Transfer within an Ionic-Liquid Force Field and Its Effect on Structure and Dynamics Youngs, Tristan G. A.; Hardacre, Christopher ChemPhysChem, Vol. 9, Issue 11 https://doi.org/10.1002/cphc.200800200	journal	August 2008
Rational design of ion force fields based on thermodynamic solvation properties Horinek, Dominik; Mamatkulov, Shavkat I.; Netz, Roland R. The Journal of Chemical Physics, Vol. 130, Issue 12 https://doi.org/10.1063/1.3081142	journal	March 2009
Solvation of lithium ions in organic electrolytes of primary lithium batteries by electrospray ionization-mass spectroscopy Fukushima, Tsuyoshi; Matsuda, Yoshiharu; Hashimoto, Hiroyuki Journal of Power Sources, Vol. 110, Issue 1 https://doi.org/10.1016/S0378-7753(02)00168-4	journal	July 2002
Conductivity and Solvation of Li ⁺ Ions of LiPF ₆ in Propylene Carbonate Solutions Kondo, Kazutaka; Sano, Mitsuru; Hiwara, Akio The Journal of Physical Chemistry B, Vol. 104, Issue 20 https://doi.org/10.1021/jp000142f	journal	May 2000
Preferential Solvation of Lithium Cations and Impacts on Oxygen Reduction in Lithium–Air Batteries Zheng, Dong; Qu, Deyu; Yang, Xiao-Qing ACS Applied Materials & Interfaces, Vol. 7, Issue 36 https://doi.org/10.1021/acsami.5b04005	journal	August 2015
Chain Folding Produces a Multilayered Morphology in a Precise Polymer: Simulations and Experiments Trigg, Edward B.; Stevens, Mark J.; Winey, Karen I. Journal of the American Chemical Society, Vol. 139, Issue 10 https://doi.org/10.1021/jacs.6b12817	journal	March 2017
Two-Dimensional Infrared Spectroscopy and Molecular Dynamics Simulation Studies of Nonaqueous Lithium Ion Battery Electrolytes Lim, Joonhyung; Lee, Kyung-Koo; Liang, Chungwen The Journal of Physical Chemistry B, Vol. 123, Issue 31 https://doi.org/10.1021/acs.jpcb.9b02026	journal	May 2019
Maximum Electrical Conductivity of Associated Lithium Salts in Solvents for Lithium–Air Batteries Horwitz, Gabriela; Rodríguez, Cristian; Factorovich, Matias The Journal of Physical Chemistry C, Vol. 123, Issue 19 https://doi.org/10.1021/acs.jpcc.9b00864	journal	April 2019
Influence of Cation Type on Ionic Aggregates in Precise Ionomers Bolintineanu, Dan S.; Stevens, Mark J.; Frischknecht, Amalie L. Macromolecules, Vol. 46, Issue 13 https://doi.org/10.1021/ma400848m	journal	June 2013
Effect of Environment on Hydrogen Bond Dynamics in Liquid Water Luzar, Alenka; Chandler, David Physical Review Letters, Vol. 76, Issue 6 https://doi.org/10.1103/PhysRevLett.76.928	journal	February 1996
Reversible multiple time scale molecular dynamics Tuckerman, M.; Berne, B. J.; Martyna, G. J. The Journal of Chemical Physics, Vol. 97, Issue 3 https://doi.org/10.1063/1.463137	journal	August 1992
Parametrization with Explicit Water of Solvents Used in Lithium-Ion Batteries: Cyclic Carbonates and Linear Ethers García-Melgarejo, Valeria; Alejandre, José; Núñez-Rojas, Edgar The Journal of Physical Chemistry B, Vol. 124, Issue 23 https://doi.org/10.1021/acs.jpcb.0c01772	journal	May 2020
Dependence of ionic association on polymer chain length in poly(ethylene oxide)-lithium triflate complexes Huang, Weiwei; Frech, Roger Polymer, Vol. 35, Issue 2 https://doi.org/10.1016/0032-3861(94)90684-X	journal	January 1994
Polarizability versus mobility: atomistic force field for ionic liquids Chaban, Vitaly Physical Chemistry Chemical Physics, Vol. 13, Issue 35 https://doi.org/10.1039/c1cp21379b	journal	January 2011
Halide, Ammonium, and Alkali Metal Ion Parameters for Modeling Aqueous Solutions Jensen, Kasper P.; Jorgensen, William L. Journal of Chemical Theory and Computation, Vol. 2, Issue 6 https://doi.org/10.1021/ct600252r	journal	August 2006
The history of polymer electrolytes Armand, M. Solid State Ionics, Vol. 69, Issue 3-4 https://doi.org/10.1016/0167-2738(94)90419-7	journal	August 1994
Accurate Static and Dynamic Properties of Liquid Electrolytes for Li-Ion Batteries from ab initio Molecular Dynamics Ganesh, P.; Jiang, De-en; Kent, P. R. C. The Journal of Physical Chemistry B, Vol. 115, Issue 12 https://doi.org/10.1021/jp2003529	journal	March 2011
Single lithium-ion conducting solid polymer electrolytes: advances and perspectives Zhang, Heng; Li, Chunmei; Piszcz, Michal Chemical Society Reviews, Vol. 46, Issue 3 https://doi.org/10.1039/C6CS00491A	journal	January 2017
Are There Stable Ion-Pairs in Room-Temperature Ionic Liquids? Molecular Dynamics Simulations of 1- n -Butyl-3-methylimidazolium Hexafluorophosphate Zhao, Wei; Leroy, Frédéric; Heggen, Berit Journal of the American Chemical Society, Vol. 131, Issue 43 https://doi.org/10.1021/ja906337p	journal	November 2009
Revisiting OPLS Force Field Parameters for Ionic Liquid Simulations Doherty, Brian; Zhong, Xiang; Gathiaka, Symon Journal of Chemical Theory and Computation, Vol. 13, Issue 12 https://doi.org/10.1021/acs.jctc.7b00520	journal	November 2017
General Trend of a Negative Li Effective Charge in Ionic Liquid Electrolytes Molinari, Nicola; Mailoa, Jonathan P.; Kozinsky, Boris The Journal of Physical Chemistry Letters, Vol. 10, Issue 10 https://doi.org/10.1021/acs.jpclett.9b00798	journal	April 2019
A force field of Li ⁺ , Na ⁺ , K ⁺ , Mg ²⁺ , Ca ²⁺ , Cl ⁻ , and SO42− in aqueous solution based on the TIP4P/2005 water model and scaled charges for the ions Zeron, I. M.; Abascal, J. L. F.; Vega, C. The Journal of Chemical Physics, Vol. 151, Issue 13 https://doi.org/10.1063/1.5121392	journal	October 2019
Polarizable Molecular Dynamics and Experiments of 1,2-Dimethoxyethane Electrolytes with Lithium and Sodium Salts: Structure and Transport Properties Liyana-Arachchi, Thilanga P.; Haskins, Justin B.; Burke, Colin M. The Journal of Physical Chemistry B, Vol. 122, Issue 36 https://doi.org/10.1021/acs.jpcb.8b03445	journal	August 2018
Insights into the Transport of Alkali Metal Ions Doped into a Plastic Crystal Electrolyte Chen, Fangfang; Pringle, Jennifer M.; Forsyth, Maria Chemistry of Materials, Vol. 27, Issue 7 https://doi.org/10.1021/acs.chemmater.5b00538	journal	March 2015
Percolated Ionic Aggregate Morphologies and Decoupled Ion Transport in Precise Sulfonated Polymers Synthesized by Ring-Opening Metathesis Polymerization Paren, Benjamin A.; Thurston, Bryce A.; Neary, William J. Macromolecules, Vol. 53, Issue 20 https://doi.org/10.1021/acs.macromol.0c01906	journal	October 2020
Navigating the minefield of battery literature Xu, Kang Communications Materials, Vol. 3, Issue 1 https://doi.org/10.1038/s43246-022-00251-5	journal	May 2022
Influence of Dielectric Constant on Ionic Transport in Polyether-Based Electrolytes Wheatle, Bill K.; Keith, Jordan R.; Mogurampelly, Santosh ACS Macro Letters, Vol. 6, Issue 12 https://doi.org/10.1021/acsmacrolett.7b00810	journal	November 2017
Microscopic dynamics in water-swollen poly(vinyl alcohol) Müller-Plathe, Florian The Journal of Chemical Physics, Vol. 108, Issue 19 https://doi.org/10.1063/1.476180	journal	May 1998
Molecular Dynamics Simulation of Li⁺BF₄^- in Ethylene Carbonate, Propylene Carbonate, and Dimethyl Carbonate Solvents Soetens, Jean-Christophe; Millot, Claude; Maigret, Bernard The Journal of Physical Chemistry A, Vol. 102, Issue 7 https://doi.org/10.1021/jp972457+	journal	January 1998
Neighborship partition of the radial distribution function for simple liquids Mazur, Stephen The Journal of Chemical Physics, Vol. 97, Issue 12 https://doi.org/10.1063/1.463302	journal	December 1992
Computational Investigation on the Role of Plasticizers on Ion Conductivity in Poly(ethylene oxide) LiTFSI Electrolytes Wu, Hui; Wick, Collin D. Macromolecules, Vol. 43, Issue 7 https://doi.org/10.1021/ma902758w	journal	April 2010
Structural and aggregate analyses of (Li salt + glyme) mixtures: the complex nature of solvate ionic liquids Shimizu, Karina; Freitas, Adilson A.; Atkin, Rob Physical Chemistry Chemical Physics, Vol. 17, Issue 34 https://doi.org/10.1039/C5CP03414K	journal	January 2015
Free Energies of Hydration and Pure Liquid Properties of Hydrocarbons from the OPLS All-Atom Model Kaminski, George; Duffy, Erin M.; Matsui, Tooru The Journal of Physical Chemistry, Vol. 98, Issue 49 https://doi.org/10.1021/j100100a043	journal	December 1994
Development of Many−Body Polarizable Force Fields for Li-Battery Applications: 2. LiTFSI-Doped Oligoether, Polyether, and Carbonate-Based Electrolytes Borodin, Oleg; Smith, Grant D. The Journal of Physical Chemistry B, Vol. 110, Issue 12 https://doi.org/10.1021/jp055080d	journal	March 2006
Solvation structure in dilute to highly concentrated electrolytes for lithium-ion and sodium-ion batteries Flores, Eibar; Åvall, Gustav; Jeschke, Steffen Electrochimica Acta, Vol. 233 https://doi.org/10.1016/j.electacta.2017.03.031	journal	April 2017
Ionic association in oligo(ethylene glycol)-lithium triflat solutions as studied by FT Raman spectroscopy Sandner, B. Solid State Ionics, Vol. 83, Issue 1-2 https://doi.org/10.1016/0167-2738(95)00223-5	journal	January 1996
Natural abundance 17O, 6Li NMR and molecular modeling studies of the solvation structures of lithium bis(fluorosulfonyl)imide/1,2-dimethoxyethane liquid electrolytes Wan, Chuan; Hu, Mary Y.; Borodin, Oleg Journal of Power Sources, Vol. 307 https://doi.org/10.1016/j.jpowsour.2015.12.120	journal	March 2016
Atomistic Simulations Predict a Surprising Variety of Morphologies in Precise Ionomers Bolintineanu, Dan S.; Stevens, Mark J.; Frischknecht, Amalie L. ACS Macro Letters, Vol. 2, Issue 3 https://doi.org/10.1021/mz300611n	journal	February 2013
Solvation Structure of Li ⁺ in Concentrated LiPF ₆ −Propylene Carbonate Solutions Kameda, Yasuo; Umebayashi, Yasuhiro; Takeuchi, Munetaka The Journal of Physical Chemistry B, Vol. 111, Issue 22 https://doi.org/10.1021/jp072597b	journal	June 2007
Scaling Atomic Partial Charges of Carbonate Solvents for Lithium Ion Solvation and Diffusion Chaudhari, Mangesh I.; Nair, Jijeesh R.; Pratt, Lawrence R. Journal of Chemical Theory and Computation, Vol. 12, Issue 12 https://doi.org/10.1021/acs.jctc.6b00824	journal	November 2016
Electrochemical measurement of transference numbers in polymer electrolytes Evans, James; Vincent, Colin A.; Bruce, Peter G. Polymer, Vol. 28, Issue 13 https://doi.org/10.1016/0032-3861(87)90394-6	journal	December 1987
Ion-water interaction potentials derived from free energy perturbation simulations Ȧqvist, Johan The Journal of Physical Chemistry, Vol. 94, Issue 21 https://doi.org/10.1021/j100384a009	journal	October 1990
Polarizable molecular interactions in condensed phase and their equivalent nonpolarizable models Leontyev, Igor V.; Stuchebrukhov, Alexei A. The Journal of Chemical Physics, Vol. 141, Issue 1 https://doi.org/10.1063/1.4884276	journal	July 2014
Complexation of lithium, sodium, and potassium carbanion pairs with polyglycol dimethyl ethers (glymes). Effect of chain length and temperature Chan, Lock Lim.; Wong, K. H.; Smid, Johannes. Journal of the American Chemical Society, Vol. 92, Issue 7 https://doi.org/10.1021/ja00710a029	journal	April 1970
Enhancing Cation Diffusion and Suppressing Anion Diffusion via Lewis-Acidic Polymer Electrolytes Savoie, Brett M.; Webb, Michael A.; Miller, Thomas F. The Journal of Physical Chemistry Letters, Vol. 8, Issue 3 https://doi.org/10.1021/acs.jpclett.6b02662	journal	January 2017
Building better batteries Armand, M.; Tarascon, J.-M. Nature, Vol. 451, Issue 7179, p. 652-657 https://doi.org/10.1038/451652a	journal	February 2008
A general purpose model for the condensed phases of water: TIP4P/2005 Abascal, J. L. F.; Vega, C. The Journal of Chemical Physics, Vol. 123, Issue 23 https://doi.org/10.1063/1.2121687	journal	December 2005
Competitive lithium solvation of linear and cyclic carbonates from quantum chemistry Borodin, Oleg; Olguin, Marco; Ganesh, P. Physical Chemistry Chemical Physics, Vol. 18, Issue 1 https://doi.org/10.1039/C5CP05121E	journal	January 2016
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
Lithium ion solvation by ethylene carbonates in lithium-ion battery electrolytes, revisited by density functional theory with the hybrid solvation model and free energy correction in solution Cui, Wei; Lansac, Yves; Lee, Hochun Physical Chemistry Chemical Physics, Vol. 18, Issue 34 https://doi.org/10.1039/C6CP01667G	journal	January 2016
Ion Transport and the True Transference Number in Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries Fong, Kara D.; Self, Julian; Diederichsen, Kyle M. ACS Central Science, Vol. 5, Issue 7 https://doi.org/10.1021/acscentsci.9b00406	journal	June 2019
Determination of Alkali and Halide Monovalent Ion Parameters for Use in Explicitly Solvated Biomolecular Simulations Joung, In Suk; Cheatham, Thomas E. The Journal of Physical Chemistry B, Vol. 112, Issue 30 https://doi.org/10.1021/jp8001614	journal	July 2008
Raman intensity study of local structure in non-aqueous electrolyte solutions—I. Cation-solvent interaction in LiClO4/ethylene carbonate Hyodo, Shi-Aki; Okabayashi, Katsuaki Electrochimica Acta, Vol. 34, Issue 11 https://doi.org/10.1016/0013-4686(89)87040-9	journal	November 1989
Why Lithium Ions Stick to Some Anions and Not Others Lytle, Tyler K.; Muralidharan, Ajay; Yethiraj, Arun The Journal of Physical Chemistry B, Vol. 125, Issue 17 https://doi.org/10.1021/acs.jpcb.1c01660	journal	April 2021
A Raman spectroscopic study of organic electrolyte solutions based on binary solvent systems of ethylene carbonate with low viscosity solvents which dissolve different lithium salts Morita, Masayuki; Asai, Yoshiko; Yoshimoto, Nobuko Journal of the Chemical Society, Faraday Transactions, Vol. 94, Issue 23 https://doi.org/10.1039/a806278a	journal	January 1998
Pulse-Gradient Spin-Echo ¹ H, ⁷ Li, and ¹⁹ F NMR Diffusion and Ionic Conductivity Measurements of 14 Organic Electrolytes Containing LiN(SO ₂ CF ₃ ) ₂ Hayamizu, Kikuko; Aihara, Yuichi; Arai, Shigemasa The Journal of Physical Chemistry B, Vol. 103, Issue 3 https://doi.org/10.1021/jp9825664	journal	January 1999
Molecular Force Field for Ionic Liquids Composed of Triflate or Bistriflylimide Anions Canongia Lopes, José N.; Pádua, Agílio A. H. The Journal of Physical Chemistry B, Vol. 108, Issue 43 https://doi.org/10.1021/jp0476545	journal	October 2004
Polymer conformation and ionic association in complexes of lithium, sodium and potassium triflate with poly (ethylene oxide) oligomers Frech, Roger; Huang, Weiwei Solid State Ionics, Vol. 72 https://doi.org/10.1016/0167-2738(94)90132-5	journal	September 1994

Similar Records

The synthesis of a new family of boron-based anion receptors and the study of their effect on ion pair dissociation and conductivity of lithium salts in nonaqueous solutions

Journal Article · 1998 · Journal of the Electrochemical Society · OSTI ID:653533

Lee, H S; Yang, X Q; Xiang, C L; +2 more

Tailoring Solvation Solvent in Localized High-Concentration Electrolytes for Lithium||Sulfurized Polyacrylonitrile

Journal Article · 2024 · ACS Applied Materials and Interfaces · OSTI ID:2341729

Kim, Ju-Myung; Gao, Peiyuan; Miao, Qiushi; +8 more

A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High-Concentration Electrolytes over Electrochemical Performance of Lithium-Ion Batteries

Journal Article · 2023 · Angewandte Chemie (International Edition) · OSTI ID:1962711

Jia, Hao; Kim, Ju‐Myung; Gao, Peiyuan; +5 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ions
lithium
molecular mechanics
oxygen
solvation

Title: Accurate Calculation of Solvation Properties of Lithium Ions in Nonaqueous Solutions

Citation Formats

References (69)

Similar Records

Related Subjects