Atomic-Scale Observations of Oxygen Release Degradation in Sulfide-Based All-Solid-State Batteries with Layered Oxide Cathodes
Atomic-Scale Observations of Oxygen Release Degradation in Sulfide-Based All-Solid-State Batteries with Layered Oxide Cathodes
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具有层状氧化物阴极的硫化物基全固态电池中氧释放降解的原子尺度观察
DOI：
10.1021/acsami.2c06950
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Kuwabara Akihide
中科院分区：
文献类型：
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作者：
Kobayashi Shunsuke;Watanabe Hideaki;Kato Takeharu;Mizuno Fuminori;Kuwabara Akihide
全固态电池在电动汽车上的应用具有相当大的潜力。了解和控制层状阴极活性材料的氧气释放对于实现全固态电池的长期运行至关重要，因为氧气释放会使阴极材料和固体电解质降解，从而引发容量退化。在本研究中，我们通过原子尺度扫描透射电子显微镜和电子能量损失谱分析验证了加速氧释放的特定界面。在linbo3涂层充分形成的界面处，氧释放被抑制。在li2s - p2s55固体电解质与Li(Ni1/3Mn1/3Ni1/3) o2阴极直接接触的界面处，氧释放形成固体电解质上的分解产物和阴极表面的反位缺陷层。这些不可逆的钝化层导致容量下降。此外，我们发现从阴极上剥离的linbo3涂层不仅物理上破坏了锂的传导路径，而且导致氧释放和阴极的劣化。这些原子尺度的见解可以通过抑制氧气释放来进一步推动全固态电池的发展。
All-solid-state batteries exhibit considerable potential for applications in electric vehicles. Understanding and controlling the oxygen release from the layered cathode active material are essential in achieving long-term operation of all-solid-state batteries because the oxygen release degrades the cathode material and the solid electrolyte, triggering capacity degradation. In this study, we verified the specific interface where the oxygen release is accelerated by atomic-scale scanning transmission electron microscopy and electron energy loss spectroscopy analyses. Oxygen release is suppressed at the interface where the LiNbO3coating layer is sufficiently formed. Decomposition products on the solid electrolyte and the antisite defect layers on the cathode surface are formed by oxygen release at the interface where the Li2S-P2S5solid electrolyte and Li(Ni1/3Mn1/3Ni1/3)O2cathode are in direct contact. These irreversible passivation layers lead to capacity degradation. In addition, we found that exfoliation of the LiNbO3coating from the cathode not only physically breaks the Li conduction path but also results in oxygen release and the deterioration of the cathode. These atomic-scale insights can further advance the development of all-solid-state batteries by suppressing oxygen release.