Solid electrolyte failure can occur through a range of different mechanisms. Electrochemical delamination at electrode and electrolyte interfaces is a prominent failure mechanism during high capacity and low N/P operating conditions, and filament formation is prevalent during a high rate and long cycle-life deposition. Interface coherency and the solid electrolyte microstructure both impact the ultimate degradation mode. The solid electrolyte microstructure, described in part by the density, periodicity, and interconnected arrangement of pores, plays a role in failure. Herein, we combine modeling, synchrotron imaging, and electrochemical experiments to systematically understand how densification and processing of solid electrolytes influence filament formation. The work reveals that the density of pores is not correlated with failure. Instead, the periodicity, size, and arrangement of pores is a driver for failure in amorphous solid electrolytes absent of grain boundaries.

中文翻译：

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固体电解质孔隙率对失效的非直观作用

固体电解质失效可能通过一系列不同的机制发生。在高容量和低 N/P 操作条件下，电极和电解质界面处的电化学分层是一个突出的失效机制，而在高速率和长循环寿命沉积过程中，细丝形成很普遍。界面相干性和固体电解质微观结构都会影响最终的降解模式。固体电解质微观结构（部分由孔隙的密度、周期性和互连排列来描述）在失效中发挥着作用。在这里，我们结合建模、同步加速器成像和电化学实验来系统地了解固体电解质的致密化和加工如何影响细丝的形成。这项工作表明，孔隙的密度与失效无关。相反，孔的周期性、尺寸和排列是缺乏晶界的非晶固体电解质失效的驱动因素。