We develop a novel microtemplate strategy to prepare unique carbon aerogels. The designed cathode materials present excellent electrochemical performance.
A carbon aerogel composite modified with ZnS (ZnS-CA) was successfully prepared through a simple in situ synthesis and used as a cathode for lithium-sulfur batteries. The nanopore ZnS-CA composites with a high specific surface area and rich mesoporous structure exhibit stronger adsorption and immobilization ability for polysulfides. The ZnS-CA/S cathode materials offer excellent electrochemical performances with lasting cycling stability and high specific capacity. In particular, the 6ZnS-CA/S sample achieves an initial capacity of 1352 mAh g À 1 at 0.2 C and maintains a high capacity of 1119 mAh g À 1 after 100 cycles. Furthermore, after 300 long cycles, it still maintains a high capacity of 730 mAh g À 1 at 1 C. These excellent performance features are attributed to the strong affinity of ZnS for Li 2 S n species, thus polysulfide shuttling can be effectively inhibited from the cathode source. Furthermore, the strong adsorption energy between ZnS and polysulfides was validated by using first-principles theory calculations, which reveals the anchoring and catalytic mechanism.
A novel net channel and N‐doping carbon aerogel (CA) are successfully prepared by an in situ and facile method via polyimide (PI) inducting for lithium–sulfur (Li–S) batteries. The PI‐directing carbon aerogel (PI‐CA) presents a cross‐linked framework, abundant porosity, and a high specific surface area. PI‐CA spheres present effective immobilizing polysulfides and high loading sulfur for a Brunauer–Emmett–Teller (BET) surface area of 2039.4 m2 g−1 and N‐doping via physical and chemical adsorption. The Li–S batteries with PI‐CA as cathode matrix exhibit excellent performance. In particular, the initial specific capacity of 2PI‐CA/S with sulfur content of 73.8 wt% delivers 1338 mAh g−1 and remains at 1102 mAh g−1 after 100 cycles at 0.2 C. The enhanced electrochemical performance mainly benefits from the mesh structure of the composite and the interaction between nitrogen and lithium polysulfide. The theoretical calculation by density functional theory (DFT) further supports the template effect of PI and the anchoring mechanism of polysulfides.
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