Molecular Engineering of Nitrile‐Based Electrolytes by Oxygen Incorporation for Fast‐Charging Lithium Metal Batteries

Nitrile‐based solvents are highly promising candidates for advanced high‐energy Li‐metal batteries (LMBs); however, their practical application is hindered by poor interfacial compatibility with Li‐metal anodes. Herein, a molecular design strategy involving the incorporation of oxygen into an organic nitrile solvent is proposed, which significantly enhances the compatibility of the modified solvent with Li‐metal anodes and enables the formulation of a non‐flammable electrolyte with improved performance for LMBs. The results demonstrate that this oxygen incorporation strategy not only enhances Li⁺ transport and interfacial reaction kinetics but also facilitates the formation of a thin and uniform solid electrolyte interphase (SEI). These improvements greatly boost the rate capability and cycling stability of LMBs, achieving a capacity retention of 81.6% after 1800 cycles at a high rate of 10 C. This work highlights the critical role of solvent molecular design in improving interfacial stability and ion transport in LMBs, offering a versatile and scalable strategy for the development of next‐generation nitrile‐based electrolytes for high‐performance LMBs.