Lithium‐ion batteries, essential for electronics and electric vehicles, predominantly use cathodes made from critical materials like cobalt. Sulfur‐based cathodes, offering a high theoretical capacity of 1675 mAh g–1 and environmental advantages due to sulfur's abundance and lower toxicity, present a more sustainable alternative. However, state‐of‐the‐art sulfur‐based electrodes do not reach the theoretical capacities, mainly because conventional electrode production relies on mixing of components into weakly coordinated slurries. Consequently, sulfur's mobility leads to battery degradation – an effect known as the “sulfur‐shuttle”. This study introduces a solution by developing a microporous, covalently‐bonded, imine‐based polymer network grown in‐situ around sulfur particles on the current collector. The polymer network (i) enables selective transport of electrolyte and Li‐ions through pores of defined size, and (ii) acts as a robust host to retain the active component of the electrode (sulfur species). The resulting cathode has superior rate performance from 0.1 C (1360 mAh g–1) to 3 C (807 mAh g–1). Demonstrating a high‐performance, sustainable sulfur cathode produced via a simple one‐pot process, our research underlines the potential of microporous polymers in addressing sulfur diffusion issues, paving the way for sulfur electrodes as viable alternatives to traditional metal‐based cathodes.

中文翻译：

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通过多孔亚胺基聚合物的原位聚合一锅法合成高容量硫阴极

锂离子电池对于电子产品和电动汽车至关重要，主要使用由钴等关键材料制成的阴极。硫基正极具有 1675 mAh g-1 的高理论容量，并且由于硫含量丰富和毒性较低而具有环境优势，是一种更可持续的替代品。然而，最先进的硫基电极并未达到理论容量，这主要是因为传统电极的生产依赖于将组分混合成弱配位浆料。因此，硫的流动性会导致电池退化——这种效应被称为“硫穿梭”。这项研究引入了一种解决方案，通过开发在集电器上的硫颗粒周围原位生长的微孔、共价键合、亚胺基聚合物网络。聚合物网络（i）能够选择性地通过指定尺寸的孔传输电解质和锂离子，并且（ii）充当强大的主体以保留电极的活性成分（硫物质）。由此产生的正极具有从 0.1 C (1360 mAh g-1) 到 3 C (807 mAh g-1) 的优异倍率性能。我们的研究展示了通过简单的一锅法生产的高性能、可持续的硫阴极，强调了微孔聚合物在解决硫扩散问题方面的潜力，为硫电极作为传统金属基阴极的可行替代品铺平了道路。