Transition from Vogel-Fulcher-Tammann to Arrhenius Ion-Conducting Behavior in Poly(Ethyl Acrylate)-Based Solid Polymer Electrolytes via Succinonitrile Plasticizer Addition

Wang, Lei; He, Yubin; Xin, Huolin L.

doi:10.1149/1945-7111/acf881

Transition from Vogel-Fulcher-Tammann to Arrhenius Ion-Conducting Behavior in Poly(Ethyl Acrylate)-Based Solid Polymer Electrolytes via Succinonitrile Plasticizer Addition

Journal Article · Fri Sep 01 04:00:00 EDT 2023 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/acf881· OSTI ID:2425527

; He, Yubin;

Solid polymer electrolytes (SPEs) offer potential advantages over liquid electrolytes, including flexibility, safety, and processability. However, they suffer from low room-temperature ionic conductivity. Recently, it has been reported a poly(ethyl acrylate) based (polyEA) SPE, by incorporating 50 wt% of succinonitrile (SN) solid plasticizer, 30 wt% of lithium salt and 5 wt% of fluoroethylene carbonate additive, which achieves a high room-temperature ionic conductivity of 1.01 × 10⁻³S cm⁻¹(Nat. Nanotechnol, 2022, 17, 768-776). This novel SPE exhibits stability against Li⁰and anodic stability up to 4.9 V vs Li⁺/Li. However, the specific mechanism responsible for its high ionic conductivity remains elusive. In this work, by adjusting the weight ratio of SN in the SPE, a transition from Vogel-Fulcher-Tammann to Arrhenius ion-conducting behavior is observed. It is demonstrated that the addition of SN leads to the gradual decoupling of Li-ion from the polymer backbone and its coordination with SN, as revealed by⁶Li solid-state nuclear magnetic resonance spectroscopy. As a result, Li-ion migration primarily occurs through SN rather than the segmental motion of the polymer backbone. Performances of the SPE in Cu||Li, Li||Li and a LiFePO₄||Li pouch cells are shown to demonstrate the commercial viability of this SPE in Li⁰-anode solid-state batteries.

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0012704

OSTI ID:: 2425527

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 9 Vol. 170; ISSN 0013-4651

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

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