Degradation Pathways of Cobalt-Free LiNiO2 Cathode in Lithium Batteries,Advanced Functional Materials

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Degradation Pathways of Cobalt-Free LiNiO2 Cathode in Lithium Batteries
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-12-21 , DOI: 10.1002/adfm.202211461
Ruijun Pan ₁ , Eunmi Jo ₁ , Zehao Cui ₁ , Arumugam Manthiram ₁

Affiliation

Electrode-electrolyte reactivity (EER) and particle cracking (PC) are considered two main causes of capacity fade in high-nickel layered oxide cathodes in lithium-based batteries. However, whether EER or PC is more critical remains debatable. Herein, the fundamental correlation between EER and PC is systematically investigated with LiNiO₂ (LNO), the ultimate cobalt-free lithium layered oxide cathode. Specifically, EER is found more critical than secondary particle cracking (SPC) in determining the cycling stability of LNO; EER leads to primary particle cracking, but mitigates SPC due to the inhibition of H2-H3 phase transformation. Two surface degradation pathways are identified for cycled LNO under low and high EERs. A common blocking surface reconstruction layer (SRL) containing electrochemically-inactive Ni₃O₄ spinel and NiO rock-salt phases is formed on LNO in an electrolyte with a high EER; in contrast, an electrochemically-active SRL featuring regions of electron- and lithium-ion-conductive LiNi₂O₄ spinel phase is formed on LNO in an electrolyte with a low EER. These findings unveil the intrinsic degradation pathways of LNO cathode and are foreseen to provide new insights into the development of lithium-based batteries with a minimized EER and a maximized service life.

中文翻译：

锂电池中无钴 LiNiO2 正极的降解途径

电极电解质反应性 (EER) 和颗粒开裂 (PC) 被认为是锂基电池中高镍层状氧化物正极容量衰减的两个主要原因。然而，EER 或 PC 哪个更重要仍有争议。在此，系统地研究了 EER 和 PC 之间的基本相关性，使用最终的无钴锂层状氧化物正极LiNiO _{2 (LNO)。}具体而言，在确定 LNO 的循环稳定性方面，EER 比二次粒子开裂 (SPC) 更为关键；EER 导致初级粒子开裂，但由于抑制 H2-H3 相变而减轻了 SPC。在低 EER 和高 EER 下，确定了循环 LNO 的两种表面降解途径。包含电化学惰性 Ni 的普通阻挡表面重建层 (SRL)₃ O ₄尖晶石和NiO岩盐相在具有高EER的电解质中在LNO上形成；相比之下，在具有低 EER 的电解质中，在 LNO 上形成了具有电子和锂离子导电 LiNi ₂ O ₄尖晶石相区域的电化学活性 SRL。这些发现揭示了 LNO 阴极的内在降解途径，预计将为开发具有最小 EER 和最长使用寿命的锂基电池提供新的见解。

更新日期：2022-12-21

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