Ultra‐Smooth and Dense Lithium Deposition Toward High‐Performance Lithium Metal Batteries
Ultra‐Smooth and Dense Lithium Deposition Toward High‐Performance Lithium Metal Batteries
复制标题
超光滑和致密的锂沉积实现高性能锂金属电池
DOI：
10.1002/adma.202210130
复制
发表时间：
2023
影响因子：
29.4
通讯作者：
Yongji Gong
中科院分区：
文献类型：
--
作者：
Zhilin Yang;Wei Liu;Qian Chen;Xingguo Wang;Weili Zhang;Qiannan Zhang;Jinghan Zuo;Yong Yao;Xiaokang Gu;Kunpeng Si;Kai Liu;Jinliang Wang;Yongji Gong
锂(Li)-金属电池(LMB)具有稳定的固体-电解液界面(SEI)和无枝晶形成，在下一代储能装置中具有巨大的潜力。在这里，垂直排列的3D Cu2S纳米片阵列是在商业铜箔的表面上制备的，它原位生成超薄的铜纳米片阵列，以降低局部电流密度和表面的Li2S层，作为一种非常优秀的人工SEI。研究发现，Li呈3D-平面沉积模型，在长期循环过程中，Li2S层可在Li的3D纳米片表面和2D平面之间可逆移动。这使得在1 mA cm-2时可以获得超光滑和致密的Li沉积，在10mAhcm-2时，≈的平均厚度为53.0µm，接近理论Li箔厚度，并且在不同的循环中高度可逆。因此，在1 mA·cm~(-2)的容量下，在醚基电解液和碳酸盐电解液中分别实现了1150个稳定的高库仑效率(CE，99.1%)循环和300个稳定的CE(98.8%)循环。当与商业阴极(LiFePO4或LiNi0.8Co0.1Mn0.1O2)相结合时，即使在−20°C的高阴极负荷、有限(或零)锂过剩和贫电解液条件下，满电池的循环性能也显著增强。
Lithium (Li)‐metal batteries (LMBs) with stable solid electrolyte interphase (SEI) and dendrite‐free formation have great potential in next‐generation energy storage devices. Here, vertically aligned 3D Cu2S nanosheet arrays are fabricated on the surface of commercial Cu foils, which in situ generate ultrathin Cu nanosheet arrays to reduce local current density and Li2S layers on the surfaces to work as an excellent artificial SEI. It is found that Li presents a 3D‐to‐planar deposition model, and Li2S layers are reversibly movable between the 3D nanosheet surface and 2D planar surface of Li during long‐term cycling. This enables ultrasmooth and dense Li deposition at 1 mA cm‐2, presenting an average thickness of ≈53.0 µm at 10 mAh cm‐2, which is close to the theoretical Li foil thickness and is highly reversible at different cycles. Thus, 1150 stable cycles with high Coulombic efficiency (CE, 99.1%) at ether‐based electrolytes and 300 stable cycles with high CE (98.8%) at carbonate electrolytes are realized in half‐cell with a capacity of 1 mAh cm‐2at 1 mA cm‐2. When coupled with commercial cathodes (LiFePO4or LiNi0.8Co0.1Mn0.1O2), the full cells present substantially enhanced cyclability under high cathode loading, limited (or zero) Li excess, and lean electrolyte conditions, even at −20 °C.