Lithium-sulfur (Li-S) battery is a promising candidate for high-energy storage devices due to its high theoretical capacity and energy density. However, both structural change and drastic phase transfer arising from irreversible and unstable conversion between S/Li₂S and polysulfides during cycling would lead rapid capacity decay and short cycle-life for lithium-sulfur battery. Herein, inspired by such principle of zippers, a self-healing zipper-like sulfur electrode was designed, which was fabricated by organo-polysulfide (-S_x-) polymer binder (PSPEG) and sulfur nanocomposite with organo-polysulfide (-S_x-) chains grafted on carbon host (CPS/S). The organo-polysulfide (-S_x-) chains on/in the carbon host or binder can not only function as redox mediator to control phase transfer between S/Li₂S and polysulfides but also act as “zipper teeth” and “zipper sliders” respectively to repair the electrode spontaneously as the sulfur electrode suffered from mechanical damages and cracks. Owing to this unique zipper-like electrode design, the structural collapse and the agglomeration of S/Li₂S were effectively suppressed. Consequently, the sulfur electrode exhibits both high capacity and excellent cycling stability, showing a specific capacity of 812 mA h g ^− 1 at 1.0 C after 300 cycles. Moreover, as the sulfur loading was increased to 7.6 mg cm⁻², the CPS/S+PSPEG electrode can still deliver a high areal capacity of 6.47 mA h cm⁻² with a low electrolyte/sulfur ratio (4.5:1, µL:mg) after 60 cycles, which verifies the feasibility of the zipper-like electrode design.

锂硫（Li-S）电池由于其高理论容量和高能量密度而成为高能量存储设备的有希望的候选者。然而，由于锂/硫电池在循环过程中S / Li ₂ S与多硫化物之间不可逆转和不稳定的转化而引起的结构变化和剧烈的相转移都会导致锂硫电池容量快速下降，循环寿命短。在此，受这种拉链原理的启发，设计了一种自修复的拉链状硫电极，该电极由有机多硫化物（-S _x-）聚合物粘合剂（PSPEG）和硫纳米复合物与有机多硫化物（-S _x）制成。-）嫁接到碳基质（CPS / S）上的链。有机多硫化物（-S _x-）碳主体或粘合剂上/之中的链不仅可以充当氧化还原介体，以控制S / Li ₂ S与多硫化物之间的相转移，还可以分别充当“拉链齿”和“拉链滑头”，自发修复电极。硫电极遭受机械损坏和裂纹。由于这种独特的拉链状电极设计，有效抑制了S / Li ₂ S的结构塌陷和结块。因此，硫电极表现出高容量和优异的循环稳定性，显示的812毫安h的比容量克 ^{-  1}在300次循环后1.0℃。此外，随着硫负载增加到7.6mg cm ^-2，CPS / S+ PSPEG电极在60个循环后仍可提供6.47 mA h cm ^-2的高面积容量，且电解质/硫的比率低（4.5：1，µL：mg），这证明了拉链状电极设计的可行性。