In-situ Construction of An Ultra-stable Conductive Composite Interface for High-Voltage All-Solid-State Lithium Metal Batteries.

In-situ Construction of An Ultra-stable Conductive Composite Interface for High-Voltage All-Solid-State Lithium Metal Batteries.
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DOI:
10.1002/anie.202000547
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发表时间:
2020-04
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通讯作者:
Kai Shi;Zipei Wan;Lu Yang;Yiwen Zhang;Yanfei Huang;Shiming Su;Heyi Xia;K. Jiang;Lu Shen;Yi Hu;Shiqi Zhang;Jing Yu;Fuzeng Ren;Yan‐Bing He;F. Kang
Kai Shi;Zipei Wan;Lu Yang;Yiwen Zhang;Yanfei Huang;Shiming Su;Heyi Xia;K. Jiang;Lu Shen;Yi Hu;Shiqi Zhang;Jing Yu;Fuzeng Ren;Yan‐Bing He;F. Kang
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作者:
Kai Shi;Zipei Wan;Lu Yang;Yiwen Zhang;Yanfei Huang;Shiming Su;Heyi Xia;K. Jiang;Lu Shen;Yi Hu;Shiqi Zhang;Jing Yu;Fuzeng Ren;Yan‐Bing He;F. Kang

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石榴石电解质与Li金属的润湿性差,导致极大的界面阻抗和Li枝晶的急剧生长。通过SnNx与金属Li在300 ℃下的转化反应,在Li6.4La3Zr1.4Ta0.6O12(LLZTO)颗粒与金属Li之间原位构建了一种新型的由Li 3 N和LiySn合金组成的超稳定导电复合界面(CCI)。LiySn合金作为LLZTO和Li金属之间的连续且坚固的桥梁可以有效地将LLZTO/Li界面电阻从4468.0 Ω降低到164.8 Ω。同时,Li 3 N作为Li离子的快速通道,可以有效地传输Li离子,并实现其在LLZTO/Li界面的均匀分布。因此,Li/LLZTO@CCI/Li对称电池稳定循环1200 h而不发生短路,并且全固态高压Li/LLZTO@CCI/LiNi0.5Co0.2Mn0.3O2电池在0.25 C下达到161.4 mAh g-1的比容量,在25 ℃下循环200次后容量留存率为92.6%,库仑效率为100.0%。
The garnet electrolyte presents poor wettability with Li metal, resulting in an extremely large interfacial impedance and drastic growth of Li dendrites. Herein, a novel ultra-stable conductive composite interface (CCI) consisting of LiySn alloy and Li3N is in-situ constructed between Li6.4La3Zr1.4Ta0.6O12 (LLZTO) pellet and Li metal by conversion reaction of SnNx with Li metal at 300 ℃. The LiySn alloy as a continuous and robust bridge between LLZTO and Li metal can effectively reduce the LLZTO/Li interfacial resistance from 4468.0 Ω to 164.8 Ω. Meanwhile, the Li3N as a fast Li ion channel can efficiently transfer Li ions and achieve their uniform distribution at the LLZTO/Li interface. Therefore, the Li/LLZTO@CCI/Li symmetric battery stably cycles for 1200 h without short circuit, and the all-solid-state high-voltage Li/LLZTO@CCI/LiNi0.5Co0.2Mn0.3O2 battery achieves a specific capacity of 161.4 mAh g-1 at 0.25 C with a capacity retention rate of 92.6 % and coulombic efficiency of 100.0% after 200 cycles at 25 ℃.