Interplay between electrochemical reactions and mechanical responses in silicon–graphite anodes and its impact on degradation

Junhyuk Moon (), Heung Chan Lee (), Heechul Jung, Shinya Wakita, Sungnim Cho, Jaegu Yoon, Joowook Lee, Atsushi Ueda, Bokkyu Choi, Sihyung Lee, Kimihiko Ito, Yoshimi Kubo, Alan Christian Lim, Jeong Gil Seo, Jungho Yoo, Seungyeon Lee, Yongnam Ham, Woonjoong Baek, Young-Gyoon Ryu () and In Taek Han
Additional contact information
Junhyuk Moon: Samsung Advanced Institute of Technology
Heung Chan Lee: Samsung Advanced Institute of Technology
Heechul Jung: Samsung Advanced Institute of Technology
Shinya Wakita: Samsung Advanced Institute of Technology
Sungnim Cho: Samsung Advanced Institute of Technology
Jaegu Yoon: Samsung Advanced Institute of Technology
Joowook Lee: Samsung Advanced Institute of Technology
Atsushi Ueda: Samsung Advanced Institute of Technology
Bokkyu Choi: Samsung Advanced Institute of Technology
Sihyung Lee: Samsung Advanced Institute of Technology
Kimihiko Ito: C4GR-GREEN, National Institute for Materials Science
Yoshimi Kubo: C4GR-GREEN, National Institute for Materials Science
Alan Christian Lim: Hanyang University
Jeong Gil Seo: Hanyang University
Jungho Yoo: National NanoFab Center
Seungyeon Lee: Samsung Advanced Institute of Technology
Yongnam Ham: Samsung Advanced Institute of Technology
Woonjoong Baek: Samsung Advanced Institute of Technology
Young-Gyoon Ryu: Samsung Advanced Institute of Technology
In Taek Han: Samsung Advanced Institute of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Durability of high-energy throughput batteries is a prerequisite for electric vehicles to penetrate the market. Despite remarkable progresses in silicon anodes with high energy densities, rapid capacity fading of full cells with silicon–graphite anodes limits their use. In this work, we unveil degradation mechanisms such as Li+ crosstalk between silicon and graphite, consequent Li+ accumulation in silicon, and capacity depression of graphite due to silicon expansion. The active material properties, i.e. silicon particle size and graphite hardness, are then modified based on these results to reduce Li+ accumulation in silicon and the subsequent degradation of the active materials in the anode. Finally, the cycling performance is tailored by designing electrodes to regulate Li+ crosstalk. The resultant full cell with an areal capacity of 6 mAh cm−2 has a cycle life of >750 cycles the volumetric energy density of 800 Wh L−1 in a commercial cell format.

Date: 2021
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DOI: 10.1038/s41467-021-22662-7

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