In Situ Thermal Polymerization of a Succinonitrile-Based Gel Polymer Electrolyte for Lithium-Oxygen Batteries

Mengyuan Song; Changhao Tian; Xintong Xu; Tao Huang; Aishui Yu

doi:10.1021/acsami.3c02155

In Situ Thermal Polymerization of a Succinonitrile-Based Gel Polymer Electrolyte for Lithium-Oxygen Batteries

ACS Appl Mater Interfaces. 2023 Apr 26;15(16):20159-20165. doi: 10.1021/acsami.3c02155. Epub 2023 Apr 13.

Authors

Mengyuan Song¹, Changhao Tian¹, Xintong Xu¹, Tao Huang², Aishui Yu¹

Affiliations

¹ Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, China.
² Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.

PMID: 37053470
DOI: 10.1021/acsami.3c02155

Abstract

For lithium-oxygen batteries (LOBs), the leakage and volatilization of a liquid electrolyte and its poor electrochemical performance are the main reasons for the slow industrial advancement. Searching for more stable electrolyte substrates and reducing the use of liquid solvents are crucial to the development of LOBs. In this work, a well-designed succinonitrile-based (SN) gel polymer electrolyte (GPE-SLFE) is prepared by in situ thermal cross-linking of an ethoxylate trimethylolpropane triacrylate (ETPTA) monomer. The continuous Li⁺ transfer channel, formed by the synergistic effect of an SN-based plastic crystal electrolyte and an ETPTA polymer network, endows the GPE-SLFE with a high room-temperature ionic conductivity (1.61 mS cm^-1 at 25 °C), a high lithium-ion transference number (t_Li+ = 0.489), and excellent long-term stability of the Li/GPE-SLFE/Li symmetric cell at a current density of 0.1 mA cm^-2 for over 220 h. Furthermore, cells with the GPE-SLFE exhibit a high discharge specific capacity of 4629.7 mAh g^-1 and achieve 40 cycles.

Keywords: continuous triple-phase boundaries; gel polymer electrolyte; in situ thermal polymerization; lithium-oxygen battery; tight interfacial contact.