Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte

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

doi:10.1021/acsami.0c03363

Molecular Design of a Highly Stable Single-Ion Conducting Polymer Gel Electrolyte

Journal Article · Fri May 15 04:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c03363· OSTI ID:1660413

Liu, Kewei ^[1]; Jiang, Sisi ^[1]; Dzwiniel, Trevor L. ^[1]; Kim, Hong-Keun ^[1]; ^[1]; Dietz Rago, Nancy L. ^[1]; ^[1]; ^[1]; Yang, Jianzhong ^[1]; Liu, Qian ^[1]; Gilbert, James ^[1]; ^[1]; Srinivasan, Venkat ^[2]; ^[1]; ^[3]

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)

Single-ion conducting (SIC) polymer electrolytes with a high Li transference number (t_Li⁺) 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 t_Li⁺ 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 t_Li⁺ 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and Cell Analysis, Modeling and Prototyping (CAMP) Facility

Sponsoring Organization:: 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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1660413

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 26 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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