Porosity Development at Li-Rich Layered Cathodes in All-Solid-State Battery during In Situ Delithiation,Nano Letters

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Porosity Development at Li-Rich Layered Cathodes in All-Solid-State Battery during In Situ Delithiation
Nano Letters ( IF 9.6 ) Pub Date : 2022-06-10 , DOI: 10.1021/acs.nanolett.2c01401
Shuang Li ₁ , Yipeng Sun ₂ , Ning Li ₃ , Wei Tong ₃ , Xueliang Sun ₂ , Charles T Black ₁ , Sooyeon Hwang ₁

Affiliation

Structural evolutions are crucial for determining the performance of high-voltage lithium, manganese-rich layered cathodes. Moreover, interface between electrode and electrolyte plays a critical role in governing ionic transfer in all-solid-state batteries. Here, we unveil two different types of porous structure in Li_1.2Ni_0.2Mn_0.6O₂ cathode with LiPON solid-state electrolyte. Nanopores are found near the cathode/electrolyte interface at pristine state, where cation mixing, phase transformation, oxygen loss, and Mn reduction are also found. In situ Li⁺ extraction induces the evolution of nanovoids, initially formed near the interface then propagated into the bulk. Despite the development of nanovoids, layered structure is conserved, suggesting the nature of nanopores and nanovoids are different and their impact would be divergent. This work demonstrates the intrinsic interfacial layer, as well as the dynamic scenario of nanovoid formation inside high-capacity layered cathode, which helps to understand the performance fading in cathodes and offers insight into the all-solid-state battery design.

中文翻译：

全固态电池中富锂层状阴极在原位脱锂过程中的孔隙率发展

结构演变对于确定高压锂、富锰层状阴极的性能至关重要。此外，电极和电解质之间的界面在控制全固态电池中的离子转移方面起着关键作用。在这里，我们在具有 LiPON 固态电解质的 Li _1.2 Ni _0.2 Mn _0.6 O ₂正极中揭示了两种不同类型的多孔结构。在原始状态下，在阴极/电解质界面附近发现了纳米孔，其中还发现了阳离子混合、相变、氧损失和 Mn 还原。原位李⁺提取诱导纳米空隙的演变，最初在界面附近形成，然后传播到本体中。尽管纳米空隙的发展，层状结构是保守的，这表明纳米孔和纳米空隙的性质是不同的，它们的影响会是不同的。这项工作展示了固有的界面层，以及在高容量层状正极内形成纳米空隙的动态场景，这有助于了解正极的性能衰减，并为全固态电池设计提供洞察力。

更新日期：2022-06-10

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