Using Data-Science Approaches to Unravel Insights for Enhanced Transport of Lithium Ions in Single-Ion Conducting Polymer Electrolytes

Zhu, Qinyu; Liu, Yifan; Shepard, Lauren B.; Bhattacharya, Debjyoti; Sinnott, Susan B.; Reinhart, Wesley F.; Cooper, Valentino R.; Kumar, Rajeev

doi:10.1021/acs.chemmater.4c02432

Title: Using Data-Science Approaches to Unravel Insights for Enhanced Transport of Lithium Ions in Single-Ion Conducting Polymer Electrolytes

Journal Article · 05 December 2024 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.4c02432 · OSTI ID:2483946

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Pennsylvania State Univ., University Park, PA (United States)

Solid polymer electrolytes have yet to achieve the desired ionic conductivity (>1 mS/cm) near room temperature required for many applications. This target implies the need to reduce the effective energy barriers for ion transport in polymer electrolytes to around 20 kJ/mol. In this work, we combine information extracted from existing experimental results with theoretical calculations to provide insights into ion transport in single-ion conductors (SICs) with a focus on lithium ion SICs. Through the analysis of temperature-dependent ionic conductivity data obtained from the literature, we evaluate different methods of extracting energy barriers for lithium transport. The traditional Arrhenius fit to the temperature-dependent ionic conductivity data indicates that the Meyer–Neldel rule holds for SICs. However, the values of the fitting parameters remain unphysical. Our modified approach based on recent work (Macromolecules 2023, 56, 15, 6051), which incorporates a fixed pre-exponential factor, reveals that the energy barriers exhibit temperature dependence over a wide range of temperatures. Using this approach, we identify anions leading to the energy barriers <30 kJ/mol, which include trifluoromethane sulfonimide (TFSI), fluoromethane sulfonimide (FSI), and boron-based organic anions. In our efforts to design the next generation of anions, which can exhibit the energy barriers <20 kJ/mol, we have performed density functional theory (DFT) based calculations to connect the chemical structures of boron-based anions via the binding energy of cation (lithium)-anion pairs with the experimentally derived effective energy barriers for ion hopping. Not only have we identified a correlation between the binding energy and the energy barriers, but we also propose a strategy to design new boron-based anions by using the correlation. This combined approach involving experiments and theoretical calculations is capable of facilitating the identification of promising new anions, which can exhibit ionic conductivity >1 mS/cm near room temperature, thereby expediting the development of novel superionic single-ion conducting polymer electrolytes.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2483946

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 24 Vol. 36; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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