All‐solid‐state batteries (ASSBs) with silicon anodes are promising candidates to overcome energy limitations of conventional lithium‐ion batteries. However, silicon undergoes severe volume changes during cycling leading to rapid degradation. In this study, a columnar silicon anode (col‐Si) fabricated by a scalable physical vapor deposition process (PVD) is integrated in all‐solid‐state batteries based on argyrodite‐type electrolyte (Li₆PS₅Cl, 3 mS cm⁻¹) and Ni‐rich layered oxide cathodes (LiNi_0.9Co_0.05Mn_0.05O₂, NCM) with a high specific capacity (210 mAh g⁻¹). The column structure exhibits a 1D breathing mechanism similar to lithium, which preserves the interface toward the electrolyte. Stable cycling is demonstrated for more than 100 cycles with a high coulombic efficiency (CE) of 99.7–99.9% in full cells with industrially relevant areal loadings of 3.5 mAh cm⁻², which is the highest value reported so far for ASSB full cells with silicon anodes. Impedance spectroscopy revealed that anode resistance is drastically reduced after first lithiation, which allows high charging currents of 0.9 mA cm⁻² at room temperature without the occurrence of dendrites and short circuits. Finally, in‐operando monitoring of pouch cells gave valuable insights into the breathing behavior of the solid‐state cell.

中文翻译：

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通过使用柱状硅阳极，使阳极间相稳定的高能​​固态电池

具有硅阳极的全固态电池（ASSB）有望克服常规锂离子电池的能源限制。但是，硅在循环过程中会发生剧烈的体积变化，从而导致快速降解。在这项研究中，柱状硅阳极（COL-Si）的制造通过一个可扩展的物理气相沉积工艺（PVD）被集成在基于硫银锗矿型电解质的全固态电池（锂₆ PS ₅氯，为3mS厘米^{- 1}）和高比容量（210 mAh g ^-1）的富镍层状氧化物阴极（LiNi _0.9 Co _0.05 Mn _0.05 O ₂，NCM））。柱状结构具有类似于锂的一维呼吸机制，可保持与电解质的界面。稳定的循环在100多个循环中得到证明，在与工业相关的平面负载为3.5 mAh cm ^-2的全电池中，库仑效率（CE）为99.7–99.9％，这是迄今为止报道的ASSB全电池的最高值硅阳极。阻抗谱显示，第一次锂化后阳极电阻急剧降低，这使得室温下0.9 mA cm ^-2的高充电电流不会出现枝晶和短路。最后，对袋状细胞进行操作中监测可以深入了解固态细胞的呼吸行为。