Ultra‐Thin Lithium Silicide Interlayer for Solid‐State Lithium‐Metal Batteries
Ultra‐Thin Lithium Silicide Interlayer for Solid‐State Lithium‐Metal Batteries
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用于固态锂金属电池的超薄硅化锂中间层
DOI：
10.1002/adma.202210835
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发表时间：
2023
影响因子：
29.4
通讯作者：
Li, Ju
中科院分区：
文献类型：
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作者：
Sung, Jaekyung;Kim, So Yeon;Harutyunyan, Avetik;Amirmaleki, Maedeh;Lee, Yoonkwang;Son, Yeonguk;Li, Ju
金属锂(LiBCC)负极和固体电解质(SE)的全固态电池正在积极发展中。然而，由于电化学和机械不稳定性，SE/LiBCC界面不稳定，阻碍了它们的运行。在这里，我们展示了一种超薄的纳米多孔混合离子电子导体中间层(≈3.25µm)，它可以调节LiBCC的沉积和剥离，作为LiOad原子形成、LiBCC成核和离子和电子在SE/LiBCC界面上远程传输的3D支架。MIEC夹层由硅化锂和碳纳米管组成，对LiBCC具有热力学稳定性，并具有高度的亲锂性能。此外，它的纳米孔(<；100 nm)将沉积的LiBCC限制在尺寸区域，在该区域LiBCC表现出由扩散变形机制控制的尺寸相关塑性。LiBCC保持足够柔软，不会机械地穿透接触的东南部。在进一步电镀后，LiBCC生长在电流收集器和MIEC中间层之间，而不是直接接触SE。结果表明，以Li3.75Si-CNT/LiBCC箔为负极，LiNi0.8Co0.1Mn0.1O2为正极的全电池，比容量为207.8 mAHg−1，首次库仑效率为92.0%，循环200次后容量保持率为88.9%(数十次循环库仑效率达99.9%)，倍率性能优异(5 C时为76%)。
All‐solid‐state batteries with metallic lithium (LiBCC) anode and solid electrolyte (SE) are under active development. However, an unstable SE/LiBCCinterface 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 LiBCCdeposition and stripping, serving as a 3D scaffold for Li0ad‐atom formation, LiBCCnucleation, and long‐range transport of ions and electrons at SE/LiBCCinterface is demonstrated. Consisting of lithium silicide and carbon nanotubes, the MIEC interlayer is thermodynamically stable against LiBCCand highly lithiophilic. Moreover, its nanopores (<100 nm) confine the deposited LiBCCto the size regime where LiBCCexhibits “smaller is much softer” size‐dependent plasticity governed by diffusive deformation mechanisms. The LiBCCthus remains soft enough not to mechanically penetrate SE in contact. Upon further plating, LiBCCgrows in between the current collector and the MIEC interlayer, not directly contacting the SE. As a result, a full‐cell having Li3.75Si‐CNT/LiBCCfoil as an anode and LiNi0.8Co0.1Mn0.1O2as 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).