Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries

• Published in: Nature communications Vol. 15; no. 1; pp. 2991 - 9
• Main Authors: Ham, So-Yeon, Sebti, Elias, Cronk, Ashley, Pennebaker, Tyler, Deysher, Grayson, Chen, Yu-Ting, Oh, Jin An Sam, Lee, Jeong Beom, Song, Min Sang, Ridley, Phillip, Tan, Darren H. S., Clément, Raphaële J., Jang, Jihyun, Meng, Ying Shirley
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 06.04.2024; Nature Publishing Group; Nature Portfolio
• Subjects: 140/131; 147/135; 147/28; 639/301/299/891; 639/4077/4079/891; Alloys; Anodes; Carbon; Cathodes; Cobalt; Cobalt oxides; Electrodes; Electrolytes; Electrolytic cells; Energy; Graphite; Humanities and Social Sciences; Lithium; Manganese; Morphology; multidisciplinary; Nickel; Polymers; Scanning electron microscopy; Science; Science (multidisciplinary); Silicon; Solid state
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-47352-y

All-solid-state batteries using Si as the anode have shown promising performance without continual solid-electrolyte interface (SEI) growth. However, the first cycle irreversible capacity loss yields low initial Coulombic efficiency (ICE) of Si, limiting the energy density. To address this, we adopt a prelithiation strategy to increase ICE and conductivity of all-solid-state Si cells. A significant increase in ICE is observed for Li 1 Si anode paired with a lithium cobalt oxide (LCO) cathode. Additionally, a comparison with lithium nickel manganese cobalt oxide (NCM) reveals that performance improvements with Si prelithiation is only applicable for full cells dominated by high anode irreversibility. With this prelithiation strategy, 15% improvement in capacity retention is achieved after 1000 cycles compared to a pure Si. With Li 1 Si, a high areal capacity of up to 10 mAh cm –2 is attained using a dry-processed LCO cathode film, suggesting that the prelithiation method may be suitable for high-loading next-generation all-solid-state batteries. All-solid-state batteries with silicon anodes have high capacities but low initial coulombic efficiencies (ICEs) because of first cycle irreversible capacity loss. Here, the authors report a prelithiation strategy to improve ICEs and reversibility.