Pang Tianlu, Wu Shufen, Wu Han, Li Xiaobao, Li Yande, Yu LiTao, Zhang Hui, Han Yong, Guo Zhi, Zhang Nian
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, China.
State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai, 200050, China.
Adv Sci (Weinh). 2025 Jun 24:e04388. doi: 10.1002/advs.202504388.
Garnet-type LiLaZrTaO (LLZO) has emerged as a highly promising solid electrolyte for next-generation Li metal batteries due to its high Li conductivity and stability against metallic lithium. However, its practical application is hindered by poor interfacial contact between Li and LLZO, as well as the persistent issue of lithium dendrite formation during cycling. In this study, a novel and efficient strategy is proposed to address these challenges by employing a room-temperature ultrasonic treatment combined with a LiMg alloy anode. The fabricated symmetrical UW-LiMg/LLZO/UW-LiMg cell exhibits a low interfacial resistance and achieves an unprecedented critical current density of 4.45 mA cm. Furthermore, these cells demonstrate excellent cycling stability, maintaining stable lithium plating/stripping for over 1000 h at a high current density of 1 mA cm with a low overpotential of ≈30 mV. The superior performance is attributed to the enhanced anode ductility achieved through Mg alloying and the formation of an ultra-stable interface layer. The all-solid-state UW-LiMg/LLZO/LiFePO battery, incorporating an ultrasonically treated alloy anode and a fluorinated cathode interface, delivers a specific capacity of 153 mAh g at 0.5 C and retains an impressive capacity retention of 90% after 200 cycles at room temperature.
石榴石型LiLaZrTaO(LLZO)因其高锂离子电导率和对金属锂的稳定性,已成为下一代锂金属电池极具前景的固体电解质。然而,锂与LLZO之间较差的界面接触以及循环过程中锂枝晶形成的持续问题阻碍了其实际应用。在本研究中,提出了一种新颖且有效的策略,通过采用室温超声处理结合锂镁合金阳极来应对这些挑战。制备的对称UW-LiMg/LLZO/UW-LiMg电池具有低界面电阻,并实现了前所未有的4.45 mA cm的临界电流密度。此外,这些电池表现出优异的循环稳定性,在1 mA cm的高电流密度下以约30 mV的低过电位保持稳定的锂电镀/剥离超过1000小时。优异的性能归因于通过镁合金化实现的阳极延展性增强以及超稳定界面层的形成。包含超声处理合金阳极和氟化阴极界面的全固态UW-LiMg/LLZO/LiFePO电池在0.5 C下的比容量为153 mAh g,在室温下200次循环后仍保持令人印象深刻的90%的容量保持率。