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Unraveling the Intra and Intercycle Interfacial Evolution of Li_6PS_5Cl-Based All-Solid-State Lithium Batteries

机译:阐明基于Li_6PS_5Cl的全固态锂电池的内部和周期间界面演化

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摘要

High-performance rechargeable all-solid-state lithium metal batteries with high energy density and enhanced safety are attractive for applications like portable electronic devices and electric vehicles. Among the various solid electrolytes, argyrodite Li6PS5Cl with high ionic conductivity and easy processability is of great interest. However, the low interface compatibility between sulfide solid electrolytes and high capacity cathodes like nickel-rich layered oxides requires many thorny issues to be resolved, such as the space charge layer (SCL) and interfacial reactions. In this work, in situ electrochemical impedance spectroscopy and in situ Raman spectroscopy measurements are performed to monitor the detailed interface evolutions in a LiNi0.8Co0.1Mn0.1O2 (NCM)/Li6PS5Cl/Li cell. Combining with ex situ characterizations including scanning electron microscopy and X-ray photoelectron spectroscopy, the evolution of the SCL and the chemical bond vibration at NCM/Li6PS5Cl interface during the early cycles is elaborated. It is found that the Li+ ion migration, which varies with the potential change, is a very significant cause of these interface behaviors. For the long-term cycling, the SCL, interfacial reactions, lithium dendrites, and chemo-mechanical failure have an integrated effect on interfaces, further deteriorating the interfacial structure and electrochemical performance. This research provides a new insight on intra and intercycle interfacial evolution of solid-state batteries.
机译:具有高能量密度和增强安全性的高性能可充电全固态锂金属电池对于便携式电子设备和电动汽车等应用具有吸引力。在各种固体电解质中,具有高离子电导率和容易加工性的亚硫酸锂Li 6 PS 5 Cl是令人关注的。但是,硫化物固体电解质和高容量阴极(如富镍层状氧化物)之间的低界面相容性需要解决许多棘手的问题,例如空间电荷层(SCL)和界面反应。在这项工作中,进行了原位电化学阻抗谱和原位拉曼光谱测量,以监测LiNi0.8Co0.1Mn0.1O2(NCM)/ Li6PS5Cl / Li电池中界面的详细演变。结合包括扫描电子显微镜和X射线光电子能谱的异位表征,阐述了早期循环中SCL的演化以及NCM / Li6PS5Cl界面处的化学键振动。发现随着电位变化而变化的Li +离子迁移是这些界面行为的非常重要的原因。对于长期循环,SCL,界面反应,锂枝晶和化学机械故障对界面具有综合影响,进一步恶化了界面结构和电化学性能。这项研究为固态电池的循环内和循环间界面演化提供了新的见识。

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