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Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination

High‐capacity cathodes (LiNi0.8Mn0.1Co0.1O2) that can boost the energy density of lithium‐ion batteries are promising candidates for vehicle electrification. However, several factors specific to high energy density materials entailing electrode reactions inhibit their application. Fluorination has shown a promising ability to combat the detrimental electrochemical performances of cathode materials, however, it remains difficult to achieve the desired functionality. Herein, a novel electrochemical fluorination (ECF) that demonstrates a promising electrochemical performance enhancement via stabilization of the cathode–electrolyte‐interphase (CEI) by forming conformal LiF is proposed. Besides LiF surface layer formation, ECF reduces the degree of fluorination‐induced Ni/Li disordering and enhances the layered structural stability as probed by X‐ray diffraction. Because of the robust CEI, ECF‐NMC811 cathodes deliver 203.0 mAh g−1 first discharge capacity at the current rate of C/10, with ≈98% capacity retention up to 100 cycles. Similarly, it delivers ≈180 mAh g−1 capacity at a 1 C rate with 86.4% capacity retention up to 200 cycles with average coulombic efficiency of > 99.5%. Comprehensive characterization with a multitude of probes reveals that ECF enhances the cycling stability of the electrode without altering bulk structure and morphology.