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

So-Yeon Ham, Elias Sebti, Ashley Cronk, Tyler Pennebaker, Grayson Deysher, Yu-Ting Chen, Jin An Sam Oh, Jeong Beom Lee, Min Sang Song, Phillip Ridley, Darren H. S. Tan, Raphaële J. Clément, Jihyun Jang () and Ying Shirley Meng ()
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So-Yeon Ham: University of California San Diego
Elias Sebti: University of California
Ashley Cronk: University of California San Diego
Tyler Pennebaker: University of California
Grayson Deysher: University of California San Diego
Yu-Ting Chen: University of California San Diego
Jin An Sam Oh: and Research (A*STAR)
Jeong Beom Lee: LG Science Park
Min Sang Song: LG Science Park
Phillip Ridley: University of California San Diego
Darren H. S. Tan: University of California San Diego
Raphaële J. Clément: University of California
Jihyun Jang: University of California San Diego
Ying Shirley Meng: University of California San Diego

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract 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 Li1Si 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 Li1Si, 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.

Date: 2024
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DOI: 10.1038/s41467-024-47352-y

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