Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte
Abstract
Single-ion conducting (SIC) polymer electrolytes with a high Li transference number (tLi+) have shown the capability to enable enhanced battery performance and safety by avoiding liquid–electrolyte leakage and suppressing Li dendrite formation. However, issues of insufficient ionic conductivity, low electrochemical stability, and poor polymer/electrode interfacial contact have greatly hindered their commercial use. In this work, a Li-containing boron-centered fluorinated SIC polymer gel electrolyte (LiBFSIE) was rationally designed to achieve a high tLi+ and high electrochemical stability. Owing to the low dissociation energy of the boron-centered anion and Li+, the as-prepared LiBFSIE exhibited an ionic conductivity of 2 × 10–4 S/cm at 35 °C, which is exclusively contributed by Li ions owing to a high tLi+ of 0.93. Both simulation and experimental approaches were applied to investigate the ion diffusion and concentration gradient in the LiBFSIE and non-cross-linked dual-ion systems. Typical rectangular Li stripping/plating voltage profiles demonstrated the uniform Li deposition assisted by LiBFSIE. The interfacial contact and electrolyte infiltration were further optimized with an in situ UV–vis-initiated polymerization method together with the electrode materials. By virtue of the high electrochemical stability of LiBFSIE, the cells achieved a promising average Coulombic efficiency of 99.95% over 200 cycles, which is higher thanmore »
- Authors:
-
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Joint Center for Energy Storage Research, Lemont, IL (United States); Argonne Collaborative Center for Energy Storage Science, Lemont, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Joint Center for Energy Storage Research, Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and Cell Analysis, Modeling and Prototyping (CAMP) Facility
- Sponsoring Org.:
- USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
- OSTI Identifier:
- 1660413
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 26; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; single ion electrolyte; polymer; lithium ion batteries; high transference number; in situ syntheses
Citation Formats
Liu, Kewei, Jiang, Sisi, Dzwiniel, Trevor L., Kim, Hong-Keun, Yu, Zhou, Dietz Rago, Nancy L., Kim, Jae Jin, Fister, Timothy T., Yang, Jianzhong, Liu, Qian, Gilbert, James, Cheng, Lei, Srinivasan, Venkat, Zhang, Zhengcheng, and Liao, Chen. Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte. United States: N. p., 2020.
Web. doi:10.1021/acsami.0c03363.
Liu, Kewei, Jiang, Sisi, Dzwiniel, Trevor L., Kim, Hong-Keun, Yu, Zhou, Dietz Rago, Nancy L., Kim, Jae Jin, Fister, Timothy T., Yang, Jianzhong, Liu, Qian, Gilbert, James, Cheng, Lei, Srinivasan, Venkat, Zhang, Zhengcheng, & Liao, Chen. Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte. United States. https://doi.org/10.1021/acsami.0c03363
Liu, Kewei, Jiang, Sisi, Dzwiniel, Trevor L., Kim, Hong-Keun, Yu, Zhou, Dietz Rago, Nancy L., Kim, Jae Jin, Fister, Timothy T., Yang, Jianzhong, Liu, Qian, Gilbert, James, Cheng, Lei, Srinivasan, Venkat, Zhang, Zhengcheng, and Liao, Chen. Fri .
"Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte". United States. https://doi.org/10.1021/acsami.0c03363. https://www.osti.gov/servlets/purl/1660413.
@article{osti_1660413,
title = {Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte},
author = {Liu, Kewei and Jiang, Sisi and Dzwiniel, Trevor L. and Kim, Hong-Keun and Yu, Zhou and Dietz Rago, Nancy L. and Kim, Jae Jin and Fister, Timothy T. and Yang, Jianzhong and Liu, Qian and Gilbert, James and Cheng, Lei and Srinivasan, Venkat and Zhang, Zhengcheng and Liao, Chen},
abstractNote = {Single-ion conducting (SIC) polymer electrolytes with a high Li transference number (tLi+) have shown the capability to enable enhanced battery performance and safety by avoiding liquid–electrolyte leakage and suppressing Li dendrite formation. However, issues of insufficient ionic conductivity, low electrochemical stability, and poor polymer/electrode interfacial contact have greatly hindered their commercial use. In this work, a Li-containing boron-centered fluorinated SIC polymer gel electrolyte (LiBFSIE) was rationally designed to achieve a high tLi+ and high electrochemical stability. Owing to the low dissociation energy of the boron-centered anion and Li+, the as-prepared LiBFSIE exhibited an ionic conductivity of 2 × 10–4 S/cm at 35 °C, which is exclusively contributed by Li ions owing to a high tLi+ of 0.93. Both simulation and experimental approaches were applied to investigate the ion diffusion and concentration gradient in the LiBFSIE and non-cross-linked dual-ion systems. Typical rectangular Li stripping/plating voltage profiles demonstrated the uniform Li deposition assisted by LiBFSIE. The interfacial contact and electrolyte infiltration were further optimized with an in situ UV–vis-initiated polymerization method together with the electrode materials. By virtue of the high electrochemical stability of LiBFSIE, the cells achieved a promising average Coulombic efficiency of 99.95% over 200 cycles, which is higher than that of liquid–electrolyte-based cells. No obvious capacity fading was observed, indicating the long-term stability of LiBFSIE for lithium metal batteries.},
doi = {10.1021/acsami.0c03363},
journal = {ACS Applied Materials and Interfaces},
number = 26,
volume = 12,
place = {United States},
year = {Fri May 15 00:00:00 EDT 2020},
month = {Fri May 15 00:00:00 EDT 2020}
}
Web of Science
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