Significantly improved cyclability of lithium manganese oxide, simultaneously inhibiting electrochemical and thermal decomposition of the electrolyte by the use of an additive

Lithium manganese oxide (LiMn₂O₄) is one of the most promising cathodes for lithium ion batteries because of its abundant resources and easy preparation. However, its poor cyclability, especially under elevated temperature, limits its application on a large scale. In this work, it is reported that the cyclability of LiMn₂O₄ can be significantly improved by applying 4-(trifluoromethyl)benzonitrile (4-TB) as an electrolyte additive. Charge/discharge tests indicate that the capacity retention of LiMn₂O₄ after 450 cycles at 1C and 55 °C in a standard electrolyte, 1 M LiPF₆ in EC/EMC/DEC (3:5:2, in weight), is improved from 19% to 69%. Further electrochemical and physical characterization demonstrates that 4-TB can, on the one hand, be electrochemically oxidized preferentially compared to the standard electrolyte, which generates a protective interphase film on LiMn₂O₄. On the other hand, 4-TB can effectively combine with protonic impurities, which inhibits the thermal decomposition of the electrolyte. This dual-functionality of 4-TB contributes to the significantly improved cyclability of LiMn₂O₄.