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 Ti⁴⁺-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_0.5Co_0.2Mn_0.3O₂ cells retains 82.4 % of its initial capacity after 600 cycles at 1C, and the high-voltage Li||LiNi_0.8Co_0.1Mn_0.1O₂ 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.