Lithium‐oxygen batteries possess an extremely high theoretical energy density, rendering them a prime candidate for next‐generation secondary batteries. However, they still face multiple problems such as huge charge polarization and poor cycle life, which lay a significant gap between laboratory research and commercial applications. In this work, we adapt 15‐crown‐5 ether (C15) as solvent to regulate the generation of discharge products in lithium‐oxygen batteries. The coronal structure endows C15 with strong affinity to Li+, firmly stabilizes the intermediate LiO2 and discharge product Li2O2. Thus, the crystalline Li2O2 is amorphized into easily decomposable amorphous products. The lithium‐oxygen batteries assembled with 0.5 M C15 electrolyte show an increased discharge capacity from 4.0 mAh cm−2 to 5.7 mAh cm−2 and a low charge overpotential of 0.88 V during the whole lifespan at 0.05 mA cm−2. The batteries with 1 M C15 electrolyte can cycle stably for 140 cycles. Furthermore, the amorphous characteristic of Li2O2 product is preserved when matched with redox mediators such as LiI, with the charge polarization further decreasing to 0.74 V over a cycle life of 190 cycles. This provides new possibilities for electrolyte design to promote Li2O2 amorphization and reduce charge overpotential in lithium‐oxygen batteries.

中文翻译：

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冠醚电解质诱导 Li2O2 非晶化，用于低极化和长寿命的 Li-O2 电池

锂氧电池具有极高的理论能量密度，使其成为下一代二次电池的主要候选者。然而，它们仍然面临着巨大的电荷极化和循环寿命差等多重问题，这使得实验室研究和商业应用之间存在很大差距。在这项工作中，我们采用15-冠-5醚（C15）作为溶剂来调节锂氧电池中放电产物的产生。冠状结构赋予C15对Li+的强亲和力，牢固地稳定了中间体LiO2和放电产物Li2O2。因此，晶体Li2O2被非晶化成易分解的非晶产物。使用 0.5 M C15 电解质组装的锂氧电池在 0.05 mA cm−2 的整个寿命期内，放电容量从 4.0 mAh cm−2 增加到 5.7 mAh cm−2，充电过电位低至 0.88 V。采用1M C15电解液的电池可稳定循环140次。此外，当与LiI等氧化还原介体配合时，Li2O2产品的非晶态特性得以保留，电荷极化在190个循环的循环寿命中进一步降低至0.74 V。这为电解液设计促进Li2O2非晶化并降低锂氧电池的充电过电势提供了新的可能性。