In situ engineered organic–inorganic bilayer solid electrolyte interphase enabling lithium metal batteries over 15,000-h lifespan

作者：Bin Zhang, K. Yue, Ke Wang, Guohao Zhao, Wenbin Huang, Li Tao, Jianmin Luo, Ying Xu, Xinyong Tao · 发表于：eScience · 年份：2025 · DOI：10.1016/j.esci.2025.100479 · 被引用次数：10 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Advanced battery technologies research

Despite significant advancements in constructing LiF-rich solid electrolyte interphases (SEIs) for high-performance lithium (Li) metal batteries, reconciling high ionic conductivity, mechanical resilience, and long-term interfacial stability persists as a critical challenge. Current approaches often fail to ensure seamless integration with the Li anode or else compromise electrolyte stability. Here, we present a dynamic in situ self-reinforcing SEI architecture achieved via selective fluorination using 1-fluorooctane, which spontaneously constructs a hybrid organic–inorganic bilayer structure during cycling. The flexible outer organic layer enhances electrolyte compatibility, while the LiF-rich inner layer ensures robust mechanical strength and promotes uniform Li-ion flux, effectively inhibiting Li dendrite growth. With these synergistic effects, the bilayer SEI provides an ultra-stable interphase with homogeneous Li deposition, yielding record-long lifespans exceeding 15,000 hours at 1 mA cm –2 and nearly 15,000 hours at 2–5 mA cm –2 in symmetric Li cells, far surpassing prior reported LiF-based Li anodes. LiFePO 4 ||Li pouch cells (with a high mass loading of 7.8 mg cm –2 and 50 μm thin Li foil) retain 80% capacity over 250 cycles at 0.5 C, demonstrating exceptional stability and practical application potential. The proposed in situ fabricated LiF-rich organic–inorganic bilayer SEI offers new perspectives to guide the practical application of high-performance Li metal batt...