Dense-Stacking Porous Conjugated Polymer as Reactive-Type Host for High-Performance Lithium Sulfur Batteries

Commercialization of the lithium-sulfur battery is hampered by bottlenecks like low sulfur loading, high cathode porosity, uncontrollable Li₂ S_x deposition and sluggish kinetics of Li₂ S activation. Herein, we developed a densely stacked redox-active hexaazatrinaphthylene (HATN) polymer with a surface area of 302 m²  g^-1 and a very high bulk density of ca. 1.60 g cm^-3 . Uniquely, HATN polymer has a similar redox potential window to S, which facilitates the binding of Li₂ S_x and its transformation chemistry within the bulky polymer host, leading to fast Li₂ S/S kinetics. The compact polymer/S electrode presents a high sulfur loading of ca. 15 mg_s  cm^-2 (200-μm thickness) with a low cathode porosity of 41 %. It delivers a high areal capacity of ca. 14 mAh cm^-2 and good cycling stability (200 cycles) at electrolyte-sulfur (E/S) ratio of 5 μL mg_s ^-1 . The assembled pouch cell delivers a cell-level high energy density of 303 Wh kg^-1 and 392 Wh L^-1 .