The use of deuterated ethyl acetate in highly concentrated electrolyte as a low-cost solvent for in situ neutron diffraction measurements of Li-ion battery electrodes
A low-cost deuterated electrolyte suitable for in situ neutron diffraction measurements of normal and high voltage Li-ion battery electrodes is reported here. Li[Ni0.4Mn0.4Co0.2]O2/graphite (NMC(442)/graphite) pouch cells filled with 1:0.1:2 (molar ratio) of lithium bis(fluorosulfonyl) imide (LiFSi):LiPF6: ethyl acetate (EA) and LiFSi:LiPF6:deuterated EA (d8-EA) electrolytes were successfully cycled between 2.8 V and 4.7 V at 40 C for 250 h without significant capacity loss, polarization growth, or gas production. The signal-to-noise ratio of neutron powder diffraction patterns taken on NMC(442) powder with a conventional deuterated organic carbonate-based electrolyte and filled with LiFSi:LiPF6:d8-EA electrolyte were virtually identical. Out of all the solvents widely available in deuterated form tested in highly-concentrated systems, EA was the only one providing a good balance between cost and charge-discharge capacity retention to 4.7 V. The use of such an electrolyte blend would half the cost of deuterated solvents needed for in situ neutron diffraction measurements of Li-ion batteries compared to conventional deuterated carbonate-based electrolytes.
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