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Title: Solvation and Dynamics of Sodium and Potassium in Ethylene Carbonate from ab Initio Molecular Dynamics Simulations

The development of sodium and potassium batteries offers a promising way to meet the scaling and cost challenges of energy storage. However, compared to Li +, several intrinsic properties of Na + and K +, including their solvation and dynamics in typical organic electrolytes utilized in battery applications, are less well-understood. Here in this paper, we report a systematic investigation of Na + and K + in ethylene carbonate (EC) using first-principles molecular dynamics simulations. Our simulations reveal significant differences in the solvation structure and dynamical properties of Na + and K + compared to Li +. We find that, in contrast to Li + which exhibits a well-defined first solvation shell, the larger Na+ and K+ ions show more disordered and flexible solvation structures. These differences in solvation were found to significantly influence the ion dynamics, leading to larger diffusion coefficients of Na + and K + compared to Li +. Our simulations also reveal a clear and interesting analog in the behavior of the ions in EC and aqueous environments, particularly in the specific ion effects on the solvent dynamics. Lastly, this work provides fundamental understanding of the intrinsic properties of Na + and K + in organicmore » electrolytes, which may ultimately influence the intercalation mechanism at the electrode–electrolyte interface and therefore battery performance, lifetime, and safety.« less
Authors:
ORCiD logo [1] ;  [1] ;  [2] ; ORCiD logo [1] ;  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physics Division
Publication Date:
Report Number(s):
LLNL-JRNL-734121
Journal ID: ISSN 1932-7447; 886030
Grant/Contract Number:
AC52-07NA27344
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 40; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE
OSTI Identifier:
1455396

Pham, Tuan Anh, Kweon, Kyoung E., Samanta, Amit, Lordi, Vincenzo, and Pask, John E.. Solvation and Dynamics of Sodium and Potassium in Ethylene Carbonate from ab Initio Molecular Dynamics Simulations. United States: N. p., Web. doi:10.1021/acs.jpcc.7b06457.
Pham, Tuan Anh, Kweon, Kyoung E., Samanta, Amit, Lordi, Vincenzo, & Pask, John E.. Solvation and Dynamics of Sodium and Potassium in Ethylene Carbonate from ab Initio Molecular Dynamics Simulations. United States. doi:10.1021/acs.jpcc.7b06457.
Pham, Tuan Anh, Kweon, Kyoung E., Samanta, Amit, Lordi, Vincenzo, and Pask, John E.. 2017. "Solvation and Dynamics of Sodium and Potassium in Ethylene Carbonate from ab Initio Molecular Dynamics Simulations". United States. doi:10.1021/acs.jpcc.7b06457. https://www.osti.gov/servlets/purl/1455396.
@article{osti_1455396,
title = {Solvation and Dynamics of Sodium and Potassium in Ethylene Carbonate from ab Initio Molecular Dynamics Simulations},
author = {Pham, Tuan Anh and Kweon, Kyoung E. and Samanta, Amit and Lordi, Vincenzo and Pask, John E.},
abstractNote = {The development of sodium and potassium batteries offers a promising way to meet the scaling and cost challenges of energy storage. However, compared to Li+, several intrinsic properties of Na+ and K+, including their solvation and dynamics in typical organic electrolytes utilized in battery applications, are less well-understood. Here in this paper, we report a systematic investigation of Na+ and K+ in ethylene carbonate (EC) using first-principles molecular dynamics simulations. Our simulations reveal significant differences in the solvation structure and dynamical properties of Na+ and K+ compared to Li+. We find that, in contrast to Li+ which exhibits a well-defined first solvation shell, the larger Na+ and K+ ions show more disordered and flexible solvation structures. These differences in solvation were found to significantly influence the ion dynamics, leading to larger diffusion coefficients of Na+ and K+ compared to Li+. Our simulations also reveal a clear and interesting analog in the behavior of the ions in EC and aqueous environments, particularly in the specific ion effects on the solvent dynamics. Lastly, this work provides fundamental understanding of the intrinsic properties of Na+ and K+ in organic electrolytes, which may ultimately influence the intercalation mechanism at the electrode–electrolyte interface and therefore battery performance, lifetime, and safety.},
doi = {10.1021/acs.jpcc.7b06457},
journal = {Journal of Physical Chemistry. C},
number = 40,
volume = 121,
place = {United States},
year = {2017},
month = {9}
}