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Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode–Electrolyte Interphase

机译：通过调节电极-电解质间相来延长高镍层状氧化物的使用寿命

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摘要

As a high-energy-density cathode for Li-ion batteries, high-Ni layered oxides, especially with ultrahigh Ni-content, suffer from short lifespans, due in part to their unstable electrode-electrolyte interphase (EEI). Herein, the cycle life of LiNi0.94Co0.06O2 is greatly extended by manipulating the EEI with a lithium bis(oxalate) (LiBOB) additive even when operated at a moderately high voltage (4.4 V vs Li/Li+). Impressively, the capacity retention can be increased from 61 to 80% after 500 cycles in a full cell paired with a graphite anode. Additionally, the presence of LiBOB enables a robust boron- and oxygen-enriched EEI that effectively inhibits continual electrolyte decomposition and offers a stable cathode surface. Moreover, the layered architecture of the cathode-electrolyte interphase (CEI) and the anode-electrolyte interphase (AEI) at the nanometer scale is revealed by time-of-flight secondary ion mass spectrometry. It is demonstrated that the cathode surface chemistry can significantly influence the AEI both chemically and physically, and AEI is modified from a thick "three-layer" to a thin "two-layer" architecture by tuning the cathode surface chemistry with LiBOB. This work presents a correlation between the EEI characteristics and battery performance and highlights the significance of manipulating surface chemistry in developing stable high-energy-density Li-ion batteries.
机译：作为锂离子电池的高能量密度阴极，高Ni层状氧化物（尤其是具有超高Ni含量的氧化物）的使用寿命短，部分原因是其不稳定的电极-电解质中间相（EEI）。在此，即使在中等高电压（4.4 V vs Li / Li +）下操作，通过使用双（草酸锂）（LiBOB）添加剂操纵EEI，也可以大大延长LiNi0.94Co0.06O2的循环寿命。令人印象深刻的是，在与石墨阳极配对的完整电池中，经过500次循环后，容量保持率可以从61％提高到80％。此外，LiBOB的存在使硼和氧的EEI健壮，有效地抑制了电解质的持续分解，并提供了稳定的阴极表面。此外，通过飞行时间二次离子质谱分析揭示了纳米级阴极-电解质间相（CEI）和阳极-电解质间相（AEI）的层状结构。结果表明，阴极表面化学性质可以在化学和物理上显着影响AEI，并且通过调整阴极表面化学性质，AEI从厚的“三层”结构变为薄的“两层”结构。 LiBOB。这项工作提出了EEI特性与电池性能之间的相关性，并强调了在开发稳定的高能​​量密度锂离子电池中操纵表面化学的重要性。

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