Recent research shows that integrating lithium metal anodes can enhance battery energy density, but the high reactivity of lithium requires handling under inert conditions to avoid degradation. To overcome this, reservoir‐free cells (RFCs) are explored, where lithium metal is electrodeposited at the current collector (CC) and solid electrolyte (SE) interface during initial charging. The electrochemical properties of electrodeposited lithium are influenced by its morphology and microstructure, which impact lithium discharge capacity and pore formation. However, little is known about how to control the microstructure of electrodeposited lithium. This work experimentally characterizes the lithium microstructure at the steel|Li6PS5Cl interface using cryogenic ion beam milling, scanning electron microscopy (SEM), and electron backscatter diffraction (EBSD), focusing on the effects of electrodeposition current density and lithium layer thickness. The results show that layer thickness, not current density, primarily governs the lithium microstructure. This “specimen thickness effect” is qualitatively described using a Monte Carlo Potts model and indicates that electrodeposited lithium metal quickly equilibrates at room temperature.

中文翻译：

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钢上电沉积的锂金属的微观结构|“无负极”固态电池中的 Li6PS5Cl 接口


最近的研究表明，集成锂金属负极可以提高电池能量密度，但锂的高反应性需要在惰性条件下处理以避免降解。为了克服这个问题，我们探索了无储液槽电池 （RFC），其中锂金属在初始充电期间在集流体 （CC） 和固体电解质 （SE） 界面处电沉积。电沉积锂的电化学性质受其形态和微观结构的影响，从而影响锂放电能力和孔隙形成。然而，关于如何控制电沉积锂的微观结构知之甚少。这项工作实验表征了钢|Li6PS5Cl 界面使用低温离子束铣削、扫描电子显微镜 （SEM） 和电子背散射衍射 （EBSD），专注于电沉积电流密度和锂层厚度的影响。结果表明，层厚度，而不是电流密度，主要控制锂的微观结构。这种“样品厚度效应”使用 Monte Carlo Potts 模型进行了定性描述，并表明电沉积的锂金属在室温下迅速平衡。