Superionic conducting vacancy-rich β-Li3N electrolyte for stable cycling of all-solid-state lithium metal batteries

作者：W.S. Li, Minsi Li, Shuo Wang, Po‐Hsiu Chien, Jing Luo, Jiamin Fu, Xiaoting Lin, Graham King, Renfei Feng, Jian Wang, Jigang Zhou, Ruying Li, Jue Liu, Yifei Mo, Tsun‐Kong Sham, Xueliang Sun · 发表于：Nature Nanotechnology · 年份：2024 · DOI：10.1038/s41565-024-01813-z · 被引用次数：120 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Inorganic Chemistry and Materials

The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm−2) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li3N SSE. This vacancy-rich β-Li3N SSE shows a high ionic conductivity of 2.14 × 10−3 S cm−1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li3N achieve breakthroughs in high critical current densities up to 45 mA cm−2 and high capacities up to 7.5 mAh cm−2, and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li3N is unveiled as intrinsic stability to lithium metal. In addition, β-Li3N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li3N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capaci...