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.

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.

Details

Title
Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries
Author
Ham, So-Yeon 1   VIAFID ORCID Logo  ; Sebti, Elias 2   VIAFID ORCID Logo  ; Cronk, Ashley 1 ; Pennebaker, Tyler 2   VIAFID ORCID Logo  ; Deysher, Grayson 1 ; Chen, Yu-Ting 1 ; Oh, Jin An Sam 3   VIAFID ORCID Logo  ; Lee, Jeong Beom 4   VIAFID ORCID Logo  ; Song, Min Sang 4 ; Ridley, Phillip 5 ; Tan, Darren H. S. 5 ; Clément, Raphaële J. 2   VIAFID ORCID Logo  ; Jang, Jihyun 6   VIAFID ORCID Logo  ; Meng, Ying Shirley 7   VIAFID ORCID Logo 

 University of California San Diego, Materials Science and Engineering Program, La Jolla, CA, USA (GRID:grid.266100.3) (ISNI:0000 0001 2107 4242) 
 University of California, Materials Department and Materials Research Laboratory, Santa Barbara, USA (GRID:grid.133342.4) (ISNI:0000 0004 1936 9676) 
 and Research (A*STAR), Insitute of Materials, Research, and Engineering, Agency of Science, Technology, Singapore, Singapore (GRID:grid.185448.4) (ISNI:0000 0004 0637 0221) 
 LG Science Park, LG Energy Solution. Ltd., Gangseo-gu, Korea (GRID:grid.185448.4) 
 University of California San Diego, Department of NanoEngineering, La Jolla, USA (GRID:grid.266100.3) (ISNI:0000 0001 2107 4242) 
 University of California San Diego, Department of NanoEngineering, La Jolla, USA (GRID:grid.266100.3) (ISNI:0000 0001 2107 4242); Sogang University, Department of Chemistry, Seoul, Republic of Korea (GRID:grid.263736.5) (ISNI:0000 0001 0286 5954) 
 University of California San Diego, Department of NanoEngineering, La Jolla, USA (GRID:grid.266100.3) (ISNI:0000 0001 2107 4242); University of Chicago, Pritzker School of Molecular Engineering, Chicago, USA (GRID:grid.170205.1) (ISNI:0000 0004 1936 7822) 
Pages
2991
Publication year
2024
Publication date
2024
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
3033950281
Copyright
© The Author(s) 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.