The utilization of layered oxides as cathode materials has significantly contributed to the advancement of the lithium-ion batteries (LIBs) with high energy density and reliability. However, the structural and interfacial instability triggered by side reactions when charged to high voltage has plagued their practical applications. Here, this work reports a novel multifunctional additive, id est, 7-Anilino-3-diethylamino-6-methyl fluoran (ADMF), which exhibits unique characteristics such as preferential adsorption, oxygen scavenging, and electropolymerization protection for high-voltage cathodes. The ADMF demonstrates the capability to ameliorate the growth of cathode-electrolyte interphase (CEI), effectively diminishing the dissolution of transition metal (TM) ions, reducing the interface impedance, and facilitating the Li⁺ transport. As a result, ADMF additive with side reaction-blocking ability significantly enhances the cycling stability of MCMB||NCM811 full-cells at 4.4 V and MCMB||LCO full-cells at 4.55 V, as evidenced by the 80% retention over 600 cycles and 87% retention after 750 cycles, respectively. These findings highlight the potential of the additive design strategy to modulate the CEI chemistry, representing a new paradigm with profound implications for the development of next-generation high-voltage LIBs.

中文翻译：

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使用多功能添加剂调节高压锂离子电池的阴极-电解质界面化学

利用层状氧化物作为正极材料极大地促进了具有高能量密度和可靠性的锂离子电池（LIB）的进步。然而，充电至高电压时副反应引发的结构和界面不稳定性一直困扰着它们的实际应用。在这里，这项工作报告了一种新型多功能添加剂，即7-苯胺基-3-二乙氨基-6-甲基荧烷（ADMF），它表现出独特的特性，如优先吸附、除氧和对高压正极的电聚合保护。ADMF 表现出改善阴极电解质界面 (CEI) 生长、有效减少过渡金属 (TM) 离子溶解、降低界面阻抗并促进 Li ⁺传输的能力。结果，具有副反应阻断能力的 ADMF 添加剂显着增强了 MCMB||NCM811 全电池在 4.4 V 下和 MCMB||LCO 全电池在 4.55 V 下的循环稳定性，600 次循环后仍保持 80% 的稳定性就证明了这一点750 次循环后的保留率分别为 87%。这些发现凸显了增材设计策略在调节 CEI 化学方面的潜力，代表了一种新范例，对下一代高压锂离子电池的开发具有深远的影响。