Stabilizing a High-Voltage Lithium-Rich Layered Oxide Cathode with a Novel Electrolyte Additive

We report a novel electrolyte additive, bis(trimethylsilyl)carbodiimide, that effectively stabilizes high-voltage lithium-rich oxide cathode. Charge/discharge tests demonstrate that even trace amounts of bis(trimethylsilyl)carbodiimide in a baseline electrolyte improve the cycling stability of this cathode significantly, either in Li-based half cells or graphite-based full cells, where the capacity retention after 200 cycles between 2 and 4.8 V at 0.5C is enhanced from 40 to 72% and 49 to 77%, respectively. Analyses using physical characterization and theoretical calculations reveal that this additive not only builds a protective film on the cathode but also eliminates detrimental hydrogen fluoride via its strong coordination with hydrogen fluoride or protons.