Fluorinated Fullerenes as Electrolyte Additives for High Ionic Conductivity Lithium-Ion Batteries.

Currently, lithium-ion batteries have an increasingly urgent need for high-performance electrolytes, and additives are highly valued for their convenience and cost-effectiveness features. In this work, the feasibilities of fullerenes and fluorinated fullerenes as typical bis(fluorosulfonyl)imide/1,2-dimethoxymethane (LiFSI/DME) electrolyte additives are rationally evaluated based on density functional theory calculations and molecular dynamic simulations. Interestingly, electronic structures of C 60 , C 60 F 2 , C 60 F 4 , C 60 F 6 , 1-C 60 F 8 , and 2-C 60 F 8 are found to be compatible with the properties required as additives. It is noted that that different numbers and positions of F atoms lead to changes in the deformation and electronic properties of fullerenes. The F atoms not only show strong covalent interactions with C cages, but also affect the C-C covalent interaction in C cages. In addition, molecular dynamic simulations unravel that the addition of trace amounts of C 60 F 4 , C 60 F 6 , and 2-C 60 F 8 can effectively enhance the Li + mobility in LiFSI/DME electrolytes. The results expand the range of applications for fullerenes and their derivatives and shed light on the research into novel additives for high-performance electrolytes.