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||LiNi0.5Co0.2Mn0.3O2 cells retains 82.4 % of its initial capacity after 600 cycles at 1C, and the high-voltage Li||LiNi0.8Co0.1Mn0.1O2 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.
Wang et al. (Mon,) studied this question.