High voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes

Ai-Min Li, Zeyi Wang, Travis P. Pollard, Weiran Zhang, Sha Tan, Tianyu Li, Chamithri Jayawardana, Sz-Chian Liou, Jiancun Rao, Brett L. Lucht, Enyuan Hu, Xiao-Qing Yang, Oleg Borodin () and Chunsheng Wang ()
Additional contact information
Ai-Min Li: University of Maryland
Zeyi Wang: University of Maryland
Travis P. Pollard: DEVCOM Army Research Laboratory
Weiran Zhang: University of Maryland
Sha Tan: Brookhaven National Laboratory
Tianyu Li: University of Maryland
Chamithri Jayawardana: Department of Chemistry, University of Rhode Island
Sz-Chian Liou: University of Maryland
Jiancun Rao: University of Maryland
Brett L. Lucht: Department of Chemistry, University of Rhode Island
Enyuan Hu: Brookhaven National Laboratory
Xiao-Qing Yang: Brookhaven National Laboratory
Oleg Borodin: DEVCOM Army Research Laboratory
Chunsheng Wang: University of Maryland

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Micro-sized silicon anodes can significantly increase the energy density of lithium-ion batteries with low cost. However, the large silicon volume changes during cycling cause cracks for both organic-inorganic interphases and silicon particles. The liquid electrolytes further penetrate the cracked silicon particles and reform the interphases, resulting in huge electrode swelling and quick capacity decay. Here we resolve these challenges by designing a high-voltage electrolyte that forms silicon-phobic interphases with weak bonding to lithium-silicon alloys. The designed electrolyte enables micro-sized silicon anodes (5 µm, 4.1 mAh cm−2) to achieve a Coulombic efficiency of 99.8% and capacity of 2175 mAh g−1 for >250 cycles and enable 100 mAh LiNi0.8Co0.15Al0.05O2 pouch full cells to deliver a high capacity of 172 mAh g−1 for 120 cycles with Coulombic efficiency of >99.9%. The high-voltage electrolytes that are capable of forming silicon-phobic interphases pave new ways for the commercialization of lithium-ion batteries using micro-sized silicon anodes.

Date: 2024
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DOI: 10.1038/s41467-024-45374-0

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