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Ultra-Thin Lithium Silicide Interlayer for Solid-State Lithium-Metal Batteries
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-19 , DOI: 10.1002/adma.202210835
Jaekyung Sung 1, 2 , So Yeon Kim 1 , Avetik Harutyunyan 3 , Maedeh Amirmaleki 1 , Yoonkwang Lee 4 , Yeonguk Son 5 , Ju Li 1
Affiliation  

All-solid-state batteries with metallic lithium (LiBCC) anode and solid electrolyte (SE) are under active development. However, an unstable SE/LiBCC interface due to electrochemical and mechanical instabilities hinders their operation. Herein, an ultra-thin nanoporous mixed ionic and electronic conductor (MIEC) interlayer (≈3.25 µm), which regulates LiBCC deposition and stripping, serving as a 3D scaffold for Li0 ad-atom formation, LiBCC nucleation, and long-range transport of ions and electrons at SE/LiBCC interface is demonstrated. Consisting of lithium silicide and carbon nanotubes, the MIEC interlayer is thermodynamically stable against LiBCC and highly lithiophilic. Moreover, its nanopores (<100 nm) confine the deposited LiBCC to the size regime where LiBCC exhibits “smaller is much softer” size-dependent plasticity governed by diffusive deformation mechanisms. The LiBCC thus remains soft enough not to mechanically penetrate SE in contact. Upon further plating, LiBCC grows in between the current collector and the MIEC interlayer, not directly contacting the SE. As a result, a full-cell having Li3.75Si-CNT/LiBCC foil as an anode and LiNi0.8Co0.1Mn0.1O2 as a cathode displays a high specific capacity of 207.8 mAh g−1, 92.0% initial Coulombic efficiency, 88.9% capacity retention after 200 cycles (Coulombic efficiency reaches 99.9% after tens of cycles), and excellent rate capability (76% at 5 C).

中文翻译:

用于固态锂金属电池的超薄锂硅化物夹层

具有金属锂 (Li BCC ) 阳极和固体电解质 (SE)的全固态电池正在积极开发中。然而,由于电化学和机械不稳定性导致不稳定的 SE/Li BCC界面阻碍了它们的运行。在此,超薄纳米多孔混合离子和电子导体 (MIEC) 夹层 (≈3.25 µm),调节 Li BCC沉积和剥离,作为 3D 支架用于 Li 0吸附原子形成、Li BCC成核和长-展示了SE/Li BCC界面处离子和电子的范围传输。MIEC 中间层由硅化锂和碳纳米管组成,对 Li BCC具有热力学稳定性和高度亲锂。此外,它的纳米孔(<100 nm)将沉积的 Li BCC限制在尺寸范围内,其中 Li BCC表现出“越小越软”的尺寸依赖性塑性,由扩散变形机制控制。因此, Li BCC保持足够柔软,不会在接触时机械地穿透 SE。进一步电镀后,Li BCC在集电器和 MIEC 夹层之间生长,不直接接触 SE。因此,具有 Li 3.75 Si-CNT/Li BCC箔作为阳极和 LiNi 0.8 Co 0.1 Mn 0.1 O 2作为阴极的全电池显示出 207.8 mAh g 的高比容量−1,初始库仑效率92.0%,200次循环后容量保持率88.9%(数十次循环后库仑效率达到99.9%),倍率性能优异(5 C时为76%)。
更新日期:2023-03-19
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