Polymer-Contraction-Enabled Topological Engineering of Graphene for 2D/3D Hybridized Li 2 S Deposition in High-Performance Li–S Batteries

Enhancing the sluggish kinetics of Li 2 S deposition and mitigating the associated electrode passivation are critical for the practical application of Li–S batteries (LSBs). However, challenges persist in simultaneously achieving fast kinetics and sufficient precipitation. Herein, we propose a polymer-contraction strategy that realizes uniform 2 D /3D hybridized Li 2 S deposition. The contraction-induced nanoscale wrinkles, with abundant tips and a distinct wavy topography, partially convert the 2D-patterned Li 2 S precipitates to a 3D model, ensuring uniform distribution and alleviated electrode passivation for complete Li 2 S precipitation. Furthermore, the polymer coatings with rich adsorptive agents effectively immobilize lithium polysulfides and accelerate ion transport, enabling rapid deposition with an adequate supply of Li ions. By optimizing Li 2 S precipitation, the batteries achieve a reversible capacity of 890 mAh g –1 at 0.1 C after 100 cycles, even at a high sulfur loading of 5 mg cm –2 and a low electrolyte/sulfur ratio of 4 μL mg –1 . Moreover, the pouch-cells show promising viability with high energy densities (297.7 Wh kg –1 and 406.0 Wh L –1 ). This work provides new insights into enhancing Li–S chemistry beyond conventional catalyst design, establishing a foundation for developing advanced LSBs.