Deep eutectic solvent-based polymer electrolyte for solid-state lithium metal batteries

Poly(ethylene) oxide(PEO)-based electrolytes have been widely studied for solid-state lithium batteries while their ionic conductivity and lithium-ion transference number still need to be further improved.Herein, using the combined experimental and theoretical approach, we demonstrate a novel, solidstate PEO-deep eutectic solvent(DES) electrolyte for the first time. We found that the in situ formation of DES can reduce the crystallinity of PEO matrix and more Li+ions can move freely owing to the weakened coordination between ether oxygens and Li-ions. Besides, we show that more Li+ions can be dissociated from Li salts in PEO-DES electrolyte using the molecular dynamics simulations. Such liquid-free PEO-DES electrolytes showed good ionic conductivity(2.1 × 10S cm) which is 160% higher than that of conventional PEO-Li TFSI(8.1 × 10S cm) electrolyte at 60 °C. Additionally, the PEO-DES electrolyte showed 136% increase of Li-ion transference number(0.33) compared with ionic liquid-doped PEO-Li TFSI(0.14) at 60 °C. Moreover, the PEO-DES exhibited good compatibility with Li metal and stable Li plating/stripping behavior with little morphology change of Li metal. This research also provides new insights into the enhancement mechanisms of novel polymer electrolytes, improving our fundamental understanding of critical challenges that have impeded the adoption of solid-state lithium metal batteries.