Catalytic Functional Domain Enables Rapid Li ⁺ Conduction in Polyether Electrolytes for Quasi-Solid-State Batteries

Polyether electrolytes (PEs) are highly promising for high-performance lithium (Li) metal batteries due to their excellent interfacial compatibility and straightforward processability. However, their practical application is hindered by intrinsically low Li + conduction, primarily resulting from insufficient free Li + concentration and sluggish Li + transport caused by strong Li + –polymer coordination. Herein, we propose an innovative “catalytic functional domain” strategy to enable fast Li + conduction in PEs for high-performance quasi-solid-state batteries (QSSBs). By incorporating Ti 4+ -based catalytic sites with weak Lewis acidity and high-dielectric property during in situ polymerization, we construct catalytic functional regions that simultaneously facilitate Li salt dissociation via anion anchoring and weaken Li + –polymer coordination through electron withdrawal. The resulting electrolyte achieves an exceptional ionic conductivity of 1.14 mS cm –1 at 25 °C and an impressive Li + transference number of 0.77. The assembled Li||Li symmetric cells demonstrate stable cycling for over 2800 h with dendrite-free Li deposition. Moreover, the Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 cells retains 82.4 % of its initial capacity after 600 cycles at 1C, and the high-voltage Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 cell sustains 403 cycles at 1C with 80% capacity retention. This work pioneers a catalytic-driven paradigm for designing advanced polymer electrolytes with accelerated Li + conduction, providing new insights toward high-performance QSSBs.