Fluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries

Yan Zhao, Tianhong Zhou, Timur Ashirov, Mario El Kazzi, Claudia Cancellieri, Lars P. H. Jeurgens, Jang Wook Choi () and Ali Coskun ()
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Yan Zhao: University of Fribourg
Tianhong Zhou: University of Fribourg
Timur Ashirov: University of Fribourg
Mario El Kazzi: Paul Scherrer Institut
Claudia Cancellieri: Laboratory for Joining Technologies and Corrosion, Swiss Federal Laboratories for Materials Science and Technology
Lars P. H. Jeurgens: Laboratory for Joining Technologies and Corrosion, Swiss Federal Laboratories for Materials Science and Technology
Jang Wook Choi: Seoul National University
Ali Coskun: University of Fribourg

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract The development of new solvents is imperative in lithium metal batteries due to the incompatibility of conventional carbonate and narrow electrochemical windows of ether-based electrolytes. Whereas the fluorinated ethers showed improved electrochemical stabilities, they can hardly solvate lithium ions. Thus, the challenge in electrolyte chemistry is to combine the high voltage stability of fluorinated ethers with high lithium ion solvation ability of ethers in a single molecule. Herein, we report a new solvent, 2,2-dimethoxy-4-(trifluoromethyl)-1,3-dioxolane (DTDL), combining a cyclic fluorinated ether with a linear ether segment to simultaneously achieve high voltage stability and tune lithium ion solvation ability and structure. High oxidation stability up to 5.5 V, large lithium ion transference number of 0.75 and stable Coulombic efficiency of 99.2% after 500 cycles proved the potential of DTDL in high-voltage lithium metal batteries. Furthermore, 20 μm thick lithium paired LiNi0.8Co0.1Mn0.1O2 full cell incorporating 2 M LiFSI-DTDL electrolyte retained 84% of the original capacity after 200 cycles at 0.5 C.

Date: 2022
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DOI: 10.1038/s41467-022-29199-3

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