Polymer-Contraction-Enabled Topological Engineering of Graphene for 2D/3D Hybridized Li₂S Deposition in High-Performance Li-S Batteries

Enhancing the sluggish kinetics of Li₂S 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 2D/3D hybridized Li₂S deposition. The contraction-induced nanoscale wrinkles, with abundant tips and a distinct wavy topography, partially convert the 2D-patterned Li₂S precipitates to a 3D model, ensuring uniform distribution and alleviated electrode passivation for complete Li₂S 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 Li₂S 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.