Healing High-Loading Sulfur Electrodes with Unprecedented Long Cycling Life: Spatial Heterogeneity Control.

Self-healing capability helps biological systems to maintain their survivability and extend their lifespan. Similarly, self-healing is also beneficial to next-generation secondary batteries because high-capacity electrode materials, especially the cathodes such as oxygen or sulfur, suffer from shortened cycle lives resulting from irreversible and unstable phase transfer. Herein, by mimicking a biological self-healing process, fibrinolysis, we introduced an extrinsic healing agent, polysulfide, to enable the stable operation of sulfur microparticle (SMiP) cathodes. An optimized capacity (∼3.7 mAh cm-2) with almost no decay after 2000 cycles at a high sulfur loading of 5.6 mg(S) cm-2 was attained. The inert SMiP is activated by the solubilization effect of polysulfides whereas the unstable phase transfer is mediated by mitigated spatial heterogeneity of polysulfides, which induces uniform nucleation and growth of solid compounds. The comprehensive understanding of the healing process, as well as of the spatial heterogeneity, could further guide the design of novel healing agents (e.g., lithium iodine) toward high-performance rechargeable batteries.