Rational Design of LixSiOy-Based Pre-SEI through Thermal-Evaporated Li-Metal Prelithiated SiOx Anode Enabling Extremely Stable and High-Rate Lithium Microbatteries

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Recently, silicon oxides families (SiOx) have been commercialized as high capacity anode materials growing rapidly owing to their natural resource abundance and low-cost.(1) However, both the poor electron/ionic conductivity, and quite low initial coulombic efficiency (ICE) (normally < 60%) limits the further development into next generation SiOx anodes. (2) To address these two critical issues, various pre-lithiation strategies have emerged and systematically investigated with significant progress.(3, 4) Here, we provide a facile approach to prelithiate SiOx films by optimizing RF power and precisely controlling Li-metal deposition to overcome the current challenges of SiOx anodes. We found a strong correlation between the surface chemical state of SiOx and the pre-formation of LixSiOy SEI layers. The optimal prelithiation strategy achieves remarkable rate performance of 72.8% at 20C, and extremely excellent long-term cycling performance of 54.2% over 5000 cycles at 10C. This study significantly promotes SiOx-based anodes development, offering a promising strategy for extreme fast-charging and long-term stability not only overcoming the limitations in microbattery but scalable to practical electrodes. Reference: Q. Mai, Chem. Soc. Rev., 48, 285 (2019). M. L. Jiao, Y. F. Wang, C. L. Ye, C. Y. Wang, W. K. Zhang and C. Liang, J. Alloy. Compd., 842, 21 (2020). R. M. Zhan, X. C. Wang, Z. H. Chen, Z. W. Seh, L. Wang and Y. M. Sun, Adv. Energy Mater., 11, 20 (2021). X. Q. Min, G. J. Xu, B. Xie, P. Guan, M. L. Sun and G. L. Cui, Energy Storage Mater., 47, 297 (2022).

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