Efficient Workflows for Detecting Li Depositions in Lithium-Ion Batteries

T. Waldmann, C. Hogrefe, Marius Flügel, Ivana Pivarníková, C. Weisenberger, Estefane Delz, Marius Bolsinger, Lioba Boveleth, Neelima Paul, M. Kasper, Max Feinauer, Robin Schäfer, Katharina Bischof, Timo Danner, Volker Knoblauch, Peter Müller‐Buschbaum, R. Gilles, A. Latz, M. Hölzle, M. Wohlfahrt‐Mehrens
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Abstract

Lithium deposition on anode surfaces can lead to fast capacity degradation and decreased safety properties of Li-ion cells. To avoid the critical aging mechanism of lithium deposition, its detection is essential. We present workflows for the efficient detection of Li deposition on electrode and cell level. The workflows are based on a variety of complementary advanced physico-chemical methods which were validated against each other for both graphite and graphite/Si electrodes: Electrochemical analysis, scanning electron microscopy, glow discharge-optical emission spectroscopy and neutron depth profiling, ex situ optical microscopy, in situ optical microscopy of cross-sectioned full cells, measurements in 3-electrode full cells, as well as 3D microstructurally resolved simulations. General considerations for workflows for analysis of battery cells and materials are discussed. The efficiency can be increased by parallel or serial execution of methods, stop criteria, and design of experiments planning. An important point in case of investigation of Li depositions are rest times during which Li can re-intercalate into the anode or react with electrolyte. Three workflows are presented to solve the questions on the occurrence of lithium deposition in an aged cell, the positions of lithium deposition in a cell, and operating conditions which avoid lithium depositions in a cell.
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检测锂离子电池中锂沉积物的高效工作流程
阳极表面的锂沉积会导致锂离子电池容量快速衰减和安全性能下降。为避免锂沉积的关键老化机制,对其进行检测至关重要。我们介绍了在电极和电池层面有效检测锂沉积的工作流程。这些工作流程基于多种互补的先进物理化学方法,并针对石墨和石墨/硅电极进行了相互验证:电化学分析、扫描电子显微镜、辉光放电-光学发射光谱和中子深度剖析、原位光学显微镜、全电池横截面原位光学显微镜、三电极全电池测量以及三维微观结构解析模拟。讨论了电池电池和材料分析工作流程的一般注意事项。可以通过并行或串行执行方法、停止标准和实验设计规划来提高效率。在研究锂沉积时,一个重要的问题是锂可以重新钙化到阳极或与电解液发生反应的静止时间。本文介绍了三个工作流程,以解决老化电池中发生锂沉积、电池中锂沉积位置以及避免电池中锂沉积的操作条件等问题。
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