Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries

Ji Chen, Xiulin Fan, Qin Li, Hongbin Yang, M. Reza Khoshi, Yaobin Xu, Sooyeon Hwang, Long Chen, Xiao Ji, Chongyin Yang, Huixin He, Chongmin Wang, Eric Garfunkel, Dong Su, Oleg Borodin () and Chunsheng Wang ()
Additional contact information
Ji Chen: University of Maryland College Park
Xiulin Fan: University of Maryland College Park
Qin Li: University of Maryland College Park
Hongbin Yang: The State University of New Jersey
M. Reza Khoshi: The State University of New Jersey
Yaobin Xu: Pacific Northwest National Laboratory
Sooyeon Hwang: Brookhaven National Laboratory
Long Chen: University of Maryland College Park
Xiao Ji: University of Maryland College Park
Chongyin Yang: University of Maryland College Park
Huixin He: The State University of New Jersey
Chongmin Wang: Pacific Northwest National Laboratory
Eric Garfunkel: The State University of New Jersey
Dong Su: Brookhaven National Laboratory
Oleg Borodin: US Army Combat Capabilities Development Command Army Research Laboratory
Chunsheng Wang: University of Maryland College Park

Nature Energy, 2020, vol. 5, issue 5, 386-397

Abstract: Abstract Lithium batteries with Si, Al or Bi microsized (>10 µm) particle anodes promise a high capacity, ease of production, low cost and low environmental impact, yet they suffer from fast degradation and a low Coulombic efficiency. Here we demonstrate that a rationally designed electrolyte (2.0 M LiPF6 in 1:1 v/v mixture of tetrahydrofuran and 2-methyltetrahydrofuran) enables 100 cycles of full cells that contain microsized Si, Al and Bi anodes with commercial LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes. Alloy anodes with areal capacities of more than 2.5 mAh cm−2 achieved >300 cycles with a high initial Coulombic efficiency of >90% and average Coulombic efficiency of >99.9%. These improvements are facilitated by the formation of a high-modulus LiF–organic bilayer interphase, in which LiF possesses a high interfacial energy with the alloy anode to accommodate plastic deformation of the lithiated alloy during cycling. This work provides a simple yet practical solution to current battery technology without any binder modification or special fabrication methods.

Date: 2020
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DOI: 10.1038/s41560-020-0601-1

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