Xu Xiangqun, Chu Shiyong, Xu Sheng, Li Haoyu, Sheng Chuanchao, Dong Mingxia, Guo Shaohua, Zhou Haoshen
College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, and Frontiers Science, Center for Critical Earth Material Cycling, Nanjing University, Nanjing, 210023, China.
Lab of Power and Energy Storage Batteries, Shenzhen Research Institute of Nanjing University, Shenzhen, 518057, China.
Angew Chem Int Ed Engl. 2025 Jan 21;64(4):e202415891. doi: 10.1002/anie.202415891. Epub 2024 Nov 6.
All-solid-state batteries (ASSBs), particularly those with Li-free anodes or even anode-free configurations, have attracted extensive attention due to high safety and energy density. However, chemical-mechanical degradation typically deteriorates the cycle life and energy of Li-free anode ASSBs with the absence of Li inventory. Here, the prelithiation agent LiFeO (LFO) coated Ni-rich layered oxide is developed as the cathode for Li-free anode ASSBs. The coated LFO acts as an interfacial protective layer to prevent the highly oxidizing Ni-rich cathode from reacting with sulfide solid-state electrolytes (SSEs), mitigating the structural degradation of Ni-rich cathodes and the decomposition of SSE, resulting in excellent cycle life. Beneficial from the coated LFO in the cathode of the Li-free anode ASSBs, the reversible capacity improves from 174.7 mAh g to 199.7 mAh g, and the capacity retention is enhanced from 33.8 % to 84.8 % after 100 cycles. Additionally, an ultrahigh energy density of 440 Wh kg, based on the mass of the composite cathode, Li-free anode, and SSE, is obtained in a Li-free anode all-solid-state pouch cell equipped with the LFO-coated cathode.
全固态电池（ASSB），尤其是那些具有无锂阳极甚至无阳极配置的电池，因其高安全性和能量密度而受到广泛关注。然而，由于缺乏锂存量，化学机械降解通常会降低无锂阳极ASSB的循环寿命和能量。在此，开发了预锂化剂LiFeO（LFO）包覆的富镍层状氧化物作为无锂阳极ASSB的阴极。包覆的LFO作为界面保护层，可防止高氧化性的富镍阴极与硫化物固态电解质（SSE）发生反应，减轻富镍阴极的结构降解和SSE的分解，从而实现优异的循环寿命。得益于无锂阳极ASSB阴极中的包覆LFO，可逆容量从174.7 mAh g提高到199.7 mAh g，100次循环后容量保持率从33.8%提高到84.8%。此外，在配备LFO包覆阴极的无锂阳极全固态软包电池中，基于复合阴极、无锂阳极和SSE的质量，获得了440 Wh kg的超高能量密度。
