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Abstract The unstable interface between Li metal and ethylene carbonate (EC)‐based electrolytes triggers continuous side reactions and uncontrolled dendrite growth, significantly impacting the lifespan of Li metal batteries (LMBs). Herein, a bipolar polymeric protective layer (BPPL) is developed using cyanoethyl (−CH 2 CH 2 C≡N) and hydroxyl (−OH) polar groups, aiming to prevent EC‐induced corrosion and facilitating rapid, uniform Li + ion transport. Hydrogen‐bonding interactions between −OH and EC facilitates the Li + desolvation process and effectively traps free EC molecules, thereby eliminating parasitic reactions. Meanwhile, the −CH 2 CH 2 C≡N group anchors TFSI − anions through ion‐dipole interactions, enhancing Li + transport and eliminating concentration polarization, ultimately suppressing the growth of Li dendrite. This BPPL enabling Li|Li cell stable cycling over 750 cycles at 10 mA cm −2 for 2 mAh cm −2 . The Li|LiNi 0.8 Mn 0.1 Co 0.1 O 2 and Li|LiFePO 4 full cells display superior electrochemical performance. The BPPL provides a practical strategy to enhanced stability and performance in LMBs application.
Deng et al. (Mon,) studied this question.