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Quadrupled Cycle Life of High-Voltage Nickel-Rich Cathodes: Understanding the Effective Thiophene-Boronic Acid-Based CEI via Operando SHINERS
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-05-24 , DOI: 10.1002/aenm.202300827
Felix Pfeiffer 1 , Diddo Diddens 1 , Matthias Weiling 1 , Lars Frankenstein 2 , Sebastian Kühn 1 , Isidora Cekic‐Laskovic 1 , Masoud Baghernejad 1
Affiliation  

Increasing the cell voltage of lithium-ion batteries (LIBs) is a straightforward approach to increasing their capacity and energy density. However, state-of-the-art cathode materials like LiNixMnyCo1-x-yO2 (NMC) suffer from severe failure mechanisms at high operating voltages, significantly degrading the performance and cycle life of the cells. Notably, an effective cathode electrolyte interphase (CEI) mitigates these failure mechanisms. Nevertheless, a deep understanding of the formation mechanisms and properties of the CEI is necessary to tailor effective interphases. This study introduces a promising electrolyte additive for high operating voltage NMC811||graphite cells. Implementing an optimized concentration of 3-thiophene boronic acid (3-Thp-BOH) significantly enhances the cells' performance and reduces capacity fading, resulting in a quadrupled cycle life and a six-times higher accumulated specific energy. Operando shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) is employed to shed light on the formation mechanism and molecular composition of CEI during cell operation, proving that the presence of the additive results in the formation of a complex 3-Thp-BOH-based polymeric CEI on the NMC811 surface. The CEI investigation is additionally supported by scanning electron microscopy and energy dispersive X-ray analysis and highly accurate quantum chemistry modeling of the suggested polymerization mechanisms.

中文翻译:

高压富镍阴极的循环寿命延长四倍:通过 Operando SHINERS 了解基于噻吩硼酸的有效 CEI

提高锂离子电池 (LIB) 的电池电压是提高其容量和能量密度的直接方法。然而,最先进的正极材料如 LiNi x Mn y Co 1-xy O 2(NMC)在高工作电压下会遭受严重的故障机制,显着降低电池的性能和循环寿命。值得注意的是,有效的阴极电解质界面(CEI)可以减轻这些故障机制。然而,深入了解 CEI 的形成机制和特性对于定制有效的界面是必要的。这项研究介绍了一种有前景的用于高工作电压 NMC811||石墨电池的电解质添加剂。采用优化浓度的 3-噻吩硼酸 (3-Thp-BOH) 可显着增强电池的性能并减少容量衰减,从而使循环寿命延长四倍,累积比能量提高六倍。Operando 壳隔离纳米粒子增强拉曼光谱 (SHINERS) 用于揭示电池运行过程中 CEI 的形成机制和分子组成,证明添加剂的存在会导致复杂的 3-Thp-BOH- 的形成。 NMC811 表面上基于聚合物 CEI。CEI 的研究还得到扫描电子显微镜和能量色散 X 射线分析以及所建议的聚合机制的高精度量子化学建模的支持。
更新日期:2023-05-24
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