A nitrile solvent structure induced stable solid electrolyte interphase for wide-temperature lithium-ion batteries
Lithium-ion batteries (LIBs) are extensively employed in various fields. Nonetheless, LIBs utilizing ethylene carbonate (EC)-based electrolytes incur capacity degradation in a wide-temperature range, which is attributable to the slow Li+ transfer kinetics at low temperatures and solvent decomposition during high-rate cycling at high temperatures. Here, we designed a novel electrolyte by substituting nitrile solvents for EC, characterized by low de-solvation energy and high ionic conductivity. The correlation between the carbon chain length of nitrile solvents with reduction stability and the Li+-solvated coordination was investigated. The results revealed that the valeronitrile (VN) solvent displayed an enhanced lowest unoccupied molecular orbital energy level and low de-solvation energy, which helped construct robust SEI interfacial layers and improved kinetics of interfacial ion transfer in wide-temperature LIBs. The VN-based electrolyte employed in graphite‖NCM523 pouch cells achieved a discharge capacity of 89.84% at a 20C rate at room temperature. Meanwhile, the cell exhibited 3C rate cycling stability even at a high temperature of 55 °C. Notably, the VN-based electrolyte exhibited a high ionic conductivity of 1.585 mS cm−1 at −50 °C. The discharge capacity of pouch cells retained 75.52% and 65.12% of their room temperature capacity at −40 °C and −50 °C, respectively. Wide-temperature-range batteries with VN-based electrolytes have the potential to be applied in various extreme environments.
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