A Caltech Library Service

Interface Structure in Li-Metal/[Pyr_(14)][TFSI]-Ionic Liquid System from Ab Initio Molecular Dynamics Simulations

Merinov, Boris V. and Zybin, Sergey V. and Naserifar, Saber and Morozov, Sergey and Oppenheim, Julius and Goddard, William A., III and Lee, Jinuk and Lee, Jae Hyun and Han, Hyea Eun and Choi, Young Cheol and Kim, Seung Ha (2019) Interface Structure in Li-Metal/[Pyr_(14)][TFSI]-Ionic Liquid System from Ab Initio Molecular Dynamics Simulations. Journal of Physical Chemistry Letters, 10 (16). pp. 4577-4586. ISSN 1948-7185.

[img] PDF - Accepted Version
See Usage Policy.

[img] PDF (Evolution of the interface structure during the simulations; pair radial distribution functions; relative Li concentration along the z-direction; initial system models) - Supplemental Material
See Usage Policy.


Use this Persistent URL to link to this item:


Ionic liquids (ILs) are promising materials for application in a new generation of Li batteries. They can be used as electrolyte or interlayer or incorporated into other materials. ILs have the ability to form a stable solid electrochemical interface (SEI), which plays an important role in protecting the Li-based electrode from oxidation and the electrolyte from extensive decomposition. Experimentally, it is hardly possible to elicit fine details of the SEI structure. To remedy this situation, we have performed a comprehensive computational study (density functional theory-based molecular dynamics) to determine the composition and structure of the SEI compact layer formed between the Li anode and [Pyr_(14)][TFSI] IL. We found that the [TFSI] anions quickly reacted with Li and decomposed, unlike the [Pyr_(14)] cations which remained stable. The obtained SEI compact layer structure is nonhomogeneous and consists of the atomized S, N, O, F, and C anions oxidized by Li atoms.

Item Type:Article
Related URLs:
URLURL TypeDescription
Merinov, Boris V.0000-0002-2783-4262
Naserifar, Saber0000-0002-1069-9789
Morozov, Sergey0000-0001-6226-5811
Oppenheim, Julius0000-0002-5988-0677
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Interface Structure in Li-Metal/[Pyr14][TFSI]-Ionic Liquid System from Ab Initio Molecular Dynamics Simulations
Additional Information:© 2019 American Chemical Society. Received: May 27, 2019; Accepted: July 25, 2019; Published: July 25, 2019. This work was supported by a research grant from LG Chem. S.M. is thankful for the support by Act 211 Government of the Russian Federation, under No. 02.A03.21.0011 and by the Supercomputer Simulation Laboratory of the South Ural State University. The authors declare no competing financial interest.
Funding AgencyGrant Number
Russian Federation02.A03.21.0011
South Ural State UniversityUNSPECIFIED
Other Numbering System:
Other Numbering System NameOther Numbering System ID
Issue or Number:16
Record Number:CaltechAUTHORS:20190729-154303026
Persistent URL:
Official Citation:Interface Structure in Li-Metal/[Pyr14][TFSI]-Ionic Liquid System from ab Initio Molecular Dynamics Simulations. Boris V. Merinov, Sergey V. Zybin, Saber Naserifar, Sergey Morozov, Julius Oppenheim, William A. Goddard, III, Jinuk Lee, Jae Hyun Lee, Hyea Eun Han, Young Cheol Choi, and Seung Ha Kim. The Journal of Physical Chemistry Letters 2019 10 (16), 4577-4586. DOI: 10.1021/acs.jpclett.9b01515
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:97498
Deposited By: Tony Diaz
Deposited On:30 Jul 2019 15:44
Last Modified:20 Feb 2020 20:12

Repository Staff Only: item control page