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Effects of High and Low Salt Concentrations in Electrolytes at Lithium–Metal Anode Surfaces Using DFT-ReaxFF Hybrid Molecular Dynamics Method

Liu, Yue and Sun, Qintao and Yu, Peiping and Wu, Yu and Xu, Liang and Yang, Hao and Xie, Miao and Cheng, Tao and Goddard, William A., III (2021) Effects of High and Low Salt Concentrations in Electrolytes at Lithium–Metal Anode Surfaces Using DFT-ReaxFF Hybrid Molecular Dynamics Method. Journal of Physical Chemistry Letters, 12 (11). pp. 2922-2929. ISSN 1948-7185. doi:10.1021/acs.jpclett.1c00279. https://resolver.caltech.edu/CaltechAUTHORS:20210317-093904113

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Abstract

Due to creating a passivated solid electrolyte interphase (SEI), high concentration (HC) electrolytes demonstrate peculiar physicochemical properties and outstanding electrochemical performance. However, the structures of such SEI remains far from clear. In this work, a hybrid abinitio and reactive molecular dynamics (HAIR) scheme is employed to investigate the concentration effect of SEI formation by simulating the reductive degradation reactions of lithium bis(fluorosulfonyl)imide (LiFSI) in 1,3 dioxalane (DOL) electrolytes at concentrations of 1 M, 4 M, and 10 M. The efficient HAIR scheme allows the simulations to reach 1 ns to predict electrolytes’ deep products at different concentrations. The simulation findings show that the most critical distinction between HC and its low concentration (LC) analogue is that anion decomposition in HC is much more incomplete when only S–F breaking is observed. These insights are important for the future development of advanced electrolytes by rational design of electrolytes.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpclett.1c00279DOIArticle
ORCID:
AuthorORCID
Yang, Hao0000-0002-8241-6231
Xie, Miao0000-0002-9797-1449
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2021 American Chemical Society. Received: February 5, 2021; Accepted: March 10, 2021; Published: March 16, 2021. T.C. and M.X. thanks the National Natural Science Foundation of China (Grants 21903058 and 22003044), the Natural Science Foundation of Jiangsu Higher Education Institutions (Grant SBK20190810), the Jiangsu Province High-Level Talents (Grant JNHB-106), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) for financial support. H.Y. thanks the China Postdoctoral Science Foundation (Grant 2019M660128) for financial support. This work was partly supported by the Collaborative Innovation Center of Suzhou Nano Science & Technology. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China21903058
National Natural Science Foundation of China22003044
Natural Science Foundation of Jiangsu Higher Education InstitutionsSBK20190810
Jiangsu Province High-Level TalentsJNHB-106
Priority Academic Program Development of Jiangsu Higher Education InstitutionsUNSPECIFIED
China Postdoctoral Science Foundation2019M660128
Suzhou Nano Science and TechnologyUNSPECIFIED
Issue or Number:11
DOI:10.1021/acs.jpclett.1c00279
Record Number:CaltechAUTHORS:20210317-093904113
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210317-093904113
Official Citation:Effects of High and Low Salt Concentrations in Electrolytes at Lithium–Metal Anode Surfaces Using DFT-ReaxFF Hybrid Molecular Dynamics Method. Yue Liu, Qintao Sun, Peiping Yu, Yu Wu, Liang Xu, Hao Yang, Miao Xie, Tao Cheng, and William A. Goddard. The Journal of Physical Chemistry Letters 2021 12 (11), 2922-2929; DOI: 10.1021/acs.jpclett.1c00279
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108466
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:19 Mar 2021 18:52
Last Modified:05 Apr 2021 19:38

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