A New Quasi-Solid Polymer Electrolyte for Next-Generation Na-O2 Batteries: Unveiling the Potential of a Polyamide-Polyether System.

Abstract

A novel quasi-solid polymer electrolyte (QSPE) composed of polyamide (PA) and polyethylene oxide (PEO), commercially known as Pebax1657, and combined with 1 M sodium bis(trifluoromethanesulfonyl)imide (NaTFSI) in diethylene glycol dimethyl ether (diglyme, DEGDME), has been investigated for sodium-oxygen (Na-O₂) batteries. Pebax1657 QSPE exhibits high ionic conductivity (6.57 × 10^-4 S cm^-1 at room temprerature - RT), an oxidation onset potential of 4.69 V versus Na/Na⁺, and an enhanced Na⁺ transference number (t_Na ^⁺ ≈ 0.40). Structural analysis (Raman spectroscopy, differential scanning calorimetry, X-ray diffraction, small-angle X-ray scattering) confirms reduced PEO crystallinity and formation of orderly nanodomains, facilitating Na⁺ transport. Long-term galvanostatic cycling in Na|Na symmetrical cells demonstrates stable overpotentials (≈80 mV) at 75 µA cm⁻² for 210 h, outperforming conventional liquid electrolytes (≈110 h). Pebax1657 QSPE enables higher discharge capacities (2.60 mAh cm⁻² at 75 µA cm⁻²; 2.11 mAh cm⁻² at 150 µA cm⁻²) with lower overpotentials (≈0.2 V). It sustains 25 cycles at 75 µA cm⁻² and 35 cycles at 150 µA cm⁻² at 0.25 mAh cm⁻², with a Coulombic Efficiency (CE) of 80-90%. Compared to the state of the art, Pebax1657 QSPE offers improved electrochemical stability, lower overpotentials, and better capacity retention. Its sustainability and versatility make it a strong candidate for Na-O₂ batteries and other energy storage applications.