Reducing the Initial Capacity Loss in High-Nickel Cathodes with a Higher Upper Cut-off Voltage Formation Cycle Protocol,ACS Energy Letters

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Reducing the Initial Capacity Loss in High-Nickel Cathodes with a Higher Upper Cut-off Voltage Formation Cycle Protocol
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-06-11 , DOI: 10.1021/acsenergylett.4c01027
Zezhou Guo ₁ , Zehao Cui ₁ , Arumugam Manthiram ₁

Affiliation

LiNiO₂-based layered oxides are regarded as promising cathode candidates for high-energy-density lithium-ion batteries. However, the large initial capacity loss (ICL) and severe electrode–electrolyte interfacial reactions significantly compromise the discharge capacity and cycle life of high-Ni cathodes. Here, we present a systemic investigation of the ICL in high-Ni cathodes by controlling the upper cutoff voltage (UCV) and dopants. It is demonstrated that the elevated ICL due to an incomplete M–H1 phase transition during discharge can be reduced via an activation step to H2–H3 phase transition at high voltages. It is shown that performing formation cycles of LiNiO₂ cells with a high UCV of 4.4 V offers significantly improved discharge capacity with minimal capacity retention penalty on cycling under a low UCV of 4.1 V. Furthermore, it is found that doping with Co reduces ICL, while other dopants, such as Mn, Al, and Mg, lead to an increase in ICL.

中文翻译：

通过较高截止电压形成循环方案减少高镍阴极的初始容量损失

LiNiO ₂ 基层状氧化物被认为是高能量密度锂离子电池的有前途的正极候选材料。然而，较大的初始容量损失（ICL）和严重的电极-电解质界面反应严重影响了高镍正极的放电容量和循环寿命。在这里，我们通过控制上限截止电压（UCV）和掺杂剂对高镍阴极中的 ICL 进行了系统研究。结果表明，由于放电过程中 M-H1 相变不完整而导致的 ICL 升高，可以通过高电压下 H2-H3 相变的激活步骤来降低。结果表明，以 4.4 V 的高 UCV 执行 LiNiO ₂ 电池的化成循环可显着提高放电容量，并且在 4.1 V 的低 UCV 下循环时容量保持损失最小。此外，还发现Co 掺杂会降低 ICL，而其他掺杂剂（例如 Mn、Al 和 Mg）会导致 ICL 增加。

更新日期：2024-06-11

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