Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization

Xia Cao, Xiaodi Ren, Lianfeng Zou, Mark H. Engelhard, William Huang, Hansen Wang, Bethany E. Matthews, Hongkyung Lee, Chaojiang Niu, Bruce W. Arey, Yi Cui, Chongmin Wang, Jie Xiao, Jun Liu, Wu Xu () and Ji-Guang Zhang ()
Additional contact information
Xia Cao: Pacific Northwest National Laboratory
Xiaodi Ren: Pacific Northwest National Laboratory
Lianfeng Zou: Pacific Northwest National Laboratory
Mark H. Engelhard: Pacific Northwest National Laboratory
William Huang: Stanford University
Hansen Wang: Stanford University
Bethany E. Matthews: Pacific Northwest National Laboratory
Hongkyung Lee: Pacific Northwest National Laboratory
Chaojiang Niu: Pacific Northwest National Laboratory
Bruce W. Arey: Pacific Northwest National Laboratory
Yi Cui: Stanford University
Chongmin Wang: Pacific Northwest National Laboratory
Jie Xiao: Pacific Northwest National Laboratory
Jun Liu: Pacific Northwest National Laboratory
Wu Xu: Pacific Northwest National Laboratory
Ji-Guang Zhang: Pacific Northwest National Laboratory

Nature Energy, 2019, vol. 4, issue 9, 796-805

Abstract: Abstract Lithium (Li) pulverization and associated large volume expansion during cycling is one of the most critical barriers for the safe operation of Li-metal batteries. Here, we report an approach to minimize the Li pulverization using an electrolyte based on a fluorinated orthoformate solvent. The solid–electrolyte interphase (SEI) formed in this electrolyte clearly exhibits a monolithic feature, which is in sharp contrast with the widely reported mosaic- or multilayer-type SEIs that are not homogeneous and could lead to uneven Li stripping/plating and fast Li and electrolyte depletion over cycling. The highly homogeneous and amorphous SEI not only prevents dendritic Li formation, but also minimizes Li loss and volumetric expansion. Furthermore, this new electrolyte strongly suppresses the phase transformation of the LiNi0.8Co0.1Mn0.1O2 cathode (from layered structure to rock salt) and stabilizes its structure. Tests of high-voltage Li||NMC811 cells show long-term cycling stability and high rate capability, as well as reduced safety concerns.

Date: 2019
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DOI: 10.1038/s41560-019-0464-5

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