Solid-State, Single-Ion Conducting, Polymer Blend Electrolytes with Enhanced Li+ Conduction, Electrochemical Stability, and Limiting Current Density

Yang, Mengying; Epps, Thomas H.

doi:10.1021/acs.chemmater.3c02389

Solid-State, Single-Ion Conducting, Polymer Blend Electrolytes with Enhanced Li⁺ Conduction, Electrochemical Stability, and Limiting Current Density

Journal Article · Thu Feb 08 00:00:00 EST 2024 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.3c02389· OSTI ID:2339829

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University of Delaware, Newark, DE (United States); University of Delaware
University of Delaware, Newark, DE (United States)

The development of solid-state polymer electrolytes with high lithium conductivity is crucial to improve lithium-ion battery performance and ameliorate the safety challenges associated with current solvent-based electrolytes. Unfortunately, sluggish polymer segmental dynamics are known to constrain conductivity enhancements in solid-state polymer electrolyte systems, limiting overall performance. In this work, a glassy single-ion-conducting polymer, poly[lithium sulfonyl(trifluoromethane sulfonyl)imide methacrylate] (PLiMTFSI), was blended with a flexible polymer, poly(oligo-oxyethylene methyl ether methacrylate) (POEM), and the impact of PLiMTFSI molecular weight and ion concentration on the thermal and ion-conducting behavior of blend electrolytes was investigated. High ionic conductivities approaching 1 × 10^-2 S/cm at 150 °C were realized in this polymer blend electrolyte system as a result of decoupling Li⁺ transport from polymer segmental dynamics. The decoupled ion transport was attributed to the packing frustration of the glassy PLiMTFSI – sufficient percolating free volume was generated to produce effective ion diffusion pathways. This decoupling was tunable as the ion transport could be altered from being closely coupled to the polymer segmental dynamics (Vogel–Tammann–Fulcher-like) to hopping (Arrhenius-like) by increasing the PLiMTFSI molecular weight and ion concentration. Moreover, the immobilized TFSI anion resulted in high Li⁺ selectivity (Li⁺ transference number = 0.9), high electrochemical stability (up to 4.7 V against Li⁺ / Li), and limiting current density of 1.8 mA/cm² (electrolyte thickness = 0.05 cm). These features suggest that this single-ion-conducting, polymer blend electrolyte might be a promising alternative to a benchmark system – salt-doped polyethylene oxide. Moreover, the above characteristics can support the battery operation at higher voltages using energy-dense Li metal anodes, with faster charging rates and enhanced energy/power densities. Altogether, the results suggest that polymer chain packing frustration can be exploited to overcome the constraints of slow polymer segmental relaxations to achieve rapid and highly selective ion transport and enhanced performance in solid-state polymer electrolytes.

View Accepted Manuscript (DOE)

Research Organization:: University of Delaware, Newark, DE (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014458

OSTI ID:: 2339829

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 4 Vol. 36; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Solid-State, Single-Ion Conducting, Polymer Blend Electrolytes with Enhanced Li+ Conduction, Electrochemical Stability, and Limiting Current Density

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