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Title: Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions

Abstract

Here, progress in understanding liquid ethylene carbonate (EC) and propylene carbonate (PC) on the basis of molecular simulation, emphasizing simple models of interatomic forces, is reviewed. Results on the bulk liquids are examined from the perspective of anticipated applications to materials for electrical energy storage devices. Preliminary results on electrochemical double-layer capacitors based on carbon nanotube forests and on model solid-electrolyte interphase (SEI) layers of lithium ion batteries are considered as examples. The basic results discussed suggest that an empirically parameterized, non-polarizable force field can reproduce experimental structural, thermodynamic, and dielectric properties of EC and PC liquids with acceptable accuracy. More sophisticated force fields might include molecular polarizability and Buckingham-model description of inter-atomic overlap repulsions as extensions to Lennard-Jones models of van der Waals interactions. Simple approaches should be similarly successful also for applications to organic molecular ions in EC/PC solutions, but the important case of Li + deserves special attention because of the particularly strong interactions of that small ion with neighboring solvent molecules. To treat the Li + ions in liquid EC/PC solutions, we identify interaction models defined by empirically scaled partial charges for ion-solvent interactions. The empirical adjustments use more basic inputs, electronic structure calculations and abmore » initio molecular dynamics simulations, and also experimental results on Li + thermodynamics and transport in EC/PC solutions. Application of such models to the mechanism of Li + transport in glassy SEI models emphasizes the advantage of long time-scale molecular dynamics studies of these non-equilibrium materials.« less

Authors:
 [1];  [2];  [2];  [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Biological and Engineering Sciences
  2. Tulane Univ., New Orleans, LA (United States). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1420188
Alternate Identifier(s):
OSTI ID: 1474049
Report Number(s):
SAND2018-10159J
Journal ID: ISSN 2365-0869; 667920
Grant/Contract Number:  
AC04-94AL85000; NA-0003525; AC02-05CH11231; 7060634; AC52-06NA25296
Resource Type:
Journal Article: Published Article
Journal Name:
Topics in Current Chemistry
Additional Journal Information:
Journal Volume: 376; Journal Issue: 2; Journal ID: ISSN 2365-0869
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Li-ion battery; Molecular dynamics simulations; Propylene carbonate; Ethylene carbonate

Citation Formats

Chaudhari, Mangesh I., Muralidharan, Ajay, Pratt, Lawrence R., and Rempe, Susan B. Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions. United States: N. p., 2018. Web. doi:10.1007/s41061-018-0187-2.
Chaudhari, Mangesh I., Muralidharan, Ajay, Pratt, Lawrence R., & Rempe, Susan B. Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions. United States. doi:10.1007/s41061-018-0187-2.
Chaudhari, Mangesh I., Muralidharan, Ajay, Pratt, Lawrence R., and Rempe, Susan B. Mon . "Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions". United States. doi:10.1007/s41061-018-0187-2.
@article{osti_1420188,
title = {Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions},
author = {Chaudhari, Mangesh I. and Muralidharan, Ajay and Pratt, Lawrence R. and Rempe, Susan B.},
abstractNote = {Here, progress in understanding liquid ethylene carbonate (EC) and propylene carbonate (PC) on the basis of molecular simulation, emphasizing simple models of interatomic forces, is reviewed. Results on the bulk liquids are examined from the perspective of anticipated applications to materials for electrical energy storage devices. Preliminary results on electrochemical double-layer capacitors based on carbon nanotube forests and on model solid-electrolyte interphase (SEI) layers of lithium ion batteries are considered as examples. The basic results discussed suggest that an empirically parameterized, non-polarizable force field can reproduce experimental structural, thermodynamic, and dielectric properties of EC and PC liquids with acceptable accuracy. More sophisticated force fields might include molecular polarizability and Buckingham-model description of inter-atomic overlap repulsions as extensions to Lennard-Jones models of van der Waals interactions. Simple approaches should be similarly successful also for applications to organic molecular ions in EC/PC solutions, but the important case of Li+ deserves special attention because of the particularly strong interactions of that small ion with neighboring solvent molecules. To treat the Li+ ions in liquid EC/PC solutions, we identify interaction models defined by empirically scaled partial charges for ion-solvent interactions. The empirical adjustments use more basic inputs, electronic structure calculations and ab initio molecular dynamics simulations, and also experimental results on Li+ thermodynamics and transport in EC/PC solutions. Application of such models to the mechanism of Li+ transport in glassy SEI models emphasizes the advantage of long time-scale molecular dynamics studies of these non-equilibrium materials.},
doi = {10.1007/s41061-018-0187-2},
journal = {Topics in Current Chemistry},
number = 2,
volume = 376,
place = {United States},
year = {Mon Feb 12 00:00:00 EST 2018},
month = {Mon Feb 12 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1007/s41061-018-0187-2

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Cited by: 1 work
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Works referenced in this record:

Carbon Nanotubes--the Route Toward Applications
journal, August 2002

  • Baughman, Ray H.; Zakhidov, Anvar A.; de Heer, Walt A.
  • Science, Vol. 297, Issue 5582, p. 787-792
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