4.8 Article

Molecular polysulfide-scavenging sulfurized-triazine polymer enable high energy density Li-S battery under lean electrolyte

Journal

ENERGY STORAGE MATERIALS
Volume 55, Issue -, Pages 225-235

Publisher

ELSEVIER
DOI: 10.1016/j.ensm.2022.11.048

Keywords

Triazine; Sulfurized polymer; Lean electrolyte; Polysulfide; Lithium-Sulfur battery

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To enhance the energy density of Li-S batteries, researchers designed STP cathodes with more than 60% sulfur, capable of cycling under a limited amount of electrolyte. These cathodes showed improved sulfur reactivity and cycle-life.
Lean electrolyte with low electrolyte/sulfur (E/S) ratio is a crucial step for the advancement of high energy density lithium-sulfur (Li-S) batteries. However, the low E/S introduces serious kinetics issues where the cell can only last for a few cycles. Here, aiming to overcome the operational constraints, we rationally design covalently grafted sulfurized-triazine polymeric (STP) cathodes housing > 60% sulfur capable of cycling under lean elec-trolyte. As-developed STP cathodes at lean E/S: 4, 6, and 8 mu L mgs-1 show improved sulfur reactivity and cycle-life, delivering 522, 574, and 601 mAh gs-1 at the 200th cycle. Further, at sulfur loading 5 mg cm-2 with E/S: 6 mu L mgs-1 tools reveal that the triazine cathode support allows covalent grafting and good wettability beneficial for facile Li ion and sulfur reactivity. As a result, the generated polysulfide is concurrently regulated in a molecularly fashion via bulk-immobilization involving abundant pyridinic-N and pyrrolic-N to confine within the electrode. Extending to construct a practical lean Li-S pouch cell with sulfur, lithium, and electrolyte accounting 53.7% cell's mass delivers an energy density of 371 Wh kg-1 that is par to the predicted values under lean electrolyte. Our study provides an invaluable resource in a potential way and future directions for developing practical high energy Li-S batteries. , the Li-S cell exhibits 588 mAh gs-1 capacity with 93% Coulombic efficiency. Experimental and modeling

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