A Sulfur-Rich Copolymer Hybrid Cathode for Anchoring Polysulfides and Accelerating Redox Reaction in Lithium Sulfur Batteries

In lithium-sulfur batteries (LSBs), sulfur-rich copolymers have attracted wide attention due to the reduced dissolution of active material and alleviated self-discharge problem through the efficient chemical interaction between polysulfide and carbon. Herein, we present an effective strategy to encapsulate sulfur-rich copolymer into NiCo2S4 encapsulated hierarchical porous N/O dual-doped graphitic carbon nanocages (GCNs), named S-DIB@NiCo2S4@PDA@rGO-GCNs. The host NiCo2S4@PDA@rGO-GCNs matrix can not only provide the “lithiophilic”-rich polar sites and tight anchored LiPSn on the N/O dual-doped GCNs surface, and “sulfphilic” NiCo2S4 electrocatalyst for accelerated sulfur electrochemistry, but also offer abundant hierarchical pores for accommodating sulfur and cushioning its volume expansion. Both of the experimental and theoretical analyses reveal the S-DIB@NiCo2S4@PDA@rGO-GCNs possesses the strong chemisorptions and catalytic ability with the synergetic mechanism, suppressing the self-discharge problem. As a proof-of-concept study, the assembled LSBs cells show excellent discharge capacities of 486 and 324 mA h g−1 at 5C and 10 C after 1000 cycles, respectively. The corresponding capacity loss rate is as low as 0.032 % and 0.030 % per cycle, respectively. Thanks to the exceptional lithiophilic and sulfiphilic characteristic, the LSBs pouch cell also demonstrates high cycling stability. The proposed hierarchical encapsulation strategy with synergetic chemisorptions and catalytic ability shows great potential for developing advanced electrodes for next-generation high-performance rechargeable batteries.