ABSTRACT
Development of efficient lithium-sulfur (Li-S) battery requires the need to develop an appropriate functional separator that allows strong facilitation and transport of lithium ions together with limited passage of polysulfides. In this work, a multifunctional separator (TB-BAA/SWCNT/PP) is developed through spin coating of a novel zwitterionic microporous polymer (TB-BAA) on the gutter layer constructed from single-walled carbon nanotubes (SWCNT), where commercially available polypropylene (PP) separator is used to act as the mechanical support. SWCNT in this study serves as the first modification layer to decrease the size of the macropores in the PP separator, while the ultrathin TB-BAA top barrier layer with the presence of zwitterionic side chains allows the creation of confined ionic channels with both lithiophilic and sulfophilic groups. Due to the presence of available chemical interactions with lithium polysulfides, selective ion transport can be foreseen through such separator. In this regard, shuttle effect that is frequently encountered in Li-S battery can be suppressed effectively via implementing the as-obtained functional separator, resulting in the creation of credible and stable sulfur electrochemistry. The TB-BAA/SWCNT/PP-based Li-S battery has been investigated to possess high cycling ability (capacity fading per cycle of 0.055% over 500 cycles at 1 C) together with decent rate capability (736.6 mAh g-1 at 3 C). In addition, a high areal capacity retention of 5.03 mAh cm-2 after 50 cycles can be also obtained under raised sulfur loading (5.4 mg cm-2).
ABSTRACT
The shuttle effect and slow redox kinetics of sulfur cathode are the most significant technical challenges to the practical application of lithium-sulfur (Li-S) battery. Herein, a novel zwitterionic covalent organic framework (ZW-COF) wrapped onto carbon nanotubes (CNTs), labeled as ZW-COF@CNT, is developed by a reversible condensation reaction of 1,3,5-benzenetricarboxaldehyde (BTA) and 3,8-diamino-6-phenylphenanthridine (DPPD) with CNTs as a template and a subsequently-one-step post-synthetic grafting reaction with 1,3-propanesultone. The experimental results showed that, after loading active material sulfur, zwitterionic ZW-COF@CNT can effectively suppress the shuttle effect of the soluble lithium polysulfides (LiPSs) in Li-S batteries, and exhibits better cycling behavior than the as-developed neutral COF@CNT. Specifically, the as-obtained ZW-COF@CNT based sulfur cathode can maintain a discharge capacity of 944 mAh/g after 100 cycles, while that of COF@CNT based sulfur cathode drops to (665 mAh/g) after 100 cycles. Moreover, the ZW-COF@CNT based sulfur cathode delivers an attractive prolonged cycling behavior with a low capacity decay rate of 0.046 % per cycle at 1 C. This work sheds new light on rational selection and design of functionalized COFs based sulfur cathode in the Li-S battery.
