Electrolyte plays a crucial role in constructing the
ionic transport
paths and oxygen diffusion routes along with maintaining the interfacial
stability based on the open working environment of lithium–oxygen
batteries. Herein, on the basis of a succinonitrile-based gel polymer
electrolyte prepared by in situ thermal-cross-linking ethoxylate trimethylolpropane
triacrylate monomer, the SLFE-5%LAGP formed by further adding Li1+x
Al
x
Ge2–x
(PO4)3 (LAGP) has high ionic
conductivity at room temperature (3.71 mS cm–1 at
25 °C), high lithium-ion transference number (t
Li+
= 0.644), and excellent long-term stability
of the Li/SLFE-5%LAGP/Li symmetric cell at a current density of 0.1
mA cm–2 for over 600 h. More importantly, LAGP can
provide adsorption sites for oxygen molecules on its surface followed
by the reduction of oxygen and the formation of Li2O2. Consequently, the cell equipped with the SLFE-5%LAGP has
an ultrahigh discharge capacity (5652.8 mAh g–1)
that exceeds the liquid electrolyte system and achieves an ultralong
stable cycling of 52 cycles. This work deepens the understanding of
the solid-state lithium–oxygen batteries through the integrated
design of electrolytes and electrodes to realize the superior solid–solid
contact interface and achieve stable long-term cycling processes.