4.8 Article

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

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 20, Pages 11359-11369

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016240

Keywords

bulky host; dense stacking; high areal capacity; high practical energy density; redox-induced polysulfide deposition

Funding

  1. NRF-CRP grant Two-Dimensional Covalent Organic Framework: Synthesis and Applications by National Research Foundation, Prime Ministers Office, Singapore [NRF-CRP16-2015-02]
  2. National Natural Science Foundation of China [21905220, 21503158]
  3. Zable Endowed Chair of Energy Technology
  4. Sustainable Power & Energy Center of UC San Diego

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The study developed a densely stacked HATN polymer as the electrode material for lithium-sulfur batteries, with high surface area and bulk density to increase sulfur loading and improve kinetics. The electrode demonstrated high energy density and cycling stability.
Commercialization of the lithium-sulfur battery is hampered by bottlenecks like low sulfur loading, high cathode porosity, uncontrollable Li2Sx deposition and sluggish kinetics of Li2S activation. Herein, we developed a densely stacked redox-active hexaazatrinaphthylene (HATN) polymer with a surface area of 302 m(2) 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 Li2Sx and its transformation chemistry within the bulky polymer host, leading to fast Li2S/S kinetics. The compact polymer/S electrode presents a high sulfur loading of ca. 15 mg(s) cm(-2) (200-mu m 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 mu L mg(s)(-1). The assembled pouch cell delivers a cell-level high energy density of 303 Wh kg(-1) and 392 Wh L-1.

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