Lithium–sulfur (Li–S) batteries hold great promise as a next‐generation battery system because of their extremely high theoretical energy density and low cost. However, ready lithium polysulfide (LiPS) diffusion and sluggish redox kinetics hamper their cyclability and rate capability. Herein, porphyrin‐derived graphene‐based nanosheets (PNG) are proposed for Li–S batteries, which are achieved by pyrolyzing a conformal and thin layer of 2D porphyrin organic framework on graphene to form carbon nanosheets with a spatially engineered nitrogen‐dopant‐enriched skin and a highly conductive skeleton. The atomic skin is decorated with fully exposed lithiophilic sites to afford strong chemisorption to LiPSs and improve electrolyte wettability, while graphene substrate provides speedy electron transport to facilitate redox kinetics of sulfur species. The use of PNG as a lightweight interlayer enables efficient operation of Li–S batteries in terms of superb cycle stability (cyclic decay rate of 0.099% during 300 cycles at 0.5 C), good rate capability (988 mAh g⁻¹ at 2.0 C), and impressive sulfur loading (areal capacity of 8.81 mAh cm⁻² at a sulfur loading of 8.9 mg cm⁻²). The distinct interfacial strategy is expected to apply to other conversion reaction batteries relying on dissolution–precipitation mechanisms and requiring interfacial charge‐ and mass‐transport‐mediation concurrently.

中文翻译：

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卟啉衍生的基于石墨烯的纳米片在锂硫电池中实现强大的多硫化物化学吸附和快速动力学

锂硫（Li–S）电池由于其极高的理论能量密度和低成本而作为下一代电池系统具有广阔的前景。然而，现成的多硫化锂（LiPS）扩散和缓慢的氧化还原动力学阻碍了它们的循环能力和速率能力。本文中，提出了用于Li–S电池的卟啉衍生的基于石墨烯的纳米片（PNG），这是通过在石墨烯上热解保形和薄薄的二维卟啉有机骨架以形成具有空间工程化的富氮掺杂剂的碳纳米片而实现的。皮肤和高导电性骨架。原子表层装饰有完全暴露的硫亲和性位点，以提供对LiPS的强化学吸附作用并改善电解质的可湿性，而石墨烯底物则提供快速的电子传输，以促进硫物质的氧化还原动力学。^-1在2.0 C），和令人印象深刻的硫负载（8.81毫安厘米面积容量^-2 8.9毫克cm的硫负载^-2）。预期独特的界面策略将适用于其他依赖于溶解-沉淀机制并同时需要界面电荷和质量传输介导的转化反应电池。