ABSTRACT Uncontrolled lithium dendrite growth and persistent electrolyte breakdown present major safety challenges, limiting the practical deployment of lithium metal batteries (LMBs). In this study, a unique organic polymer (Ni‐HAT CN), rich in lithiophilic sites and cationic groups, is designed as a protective layer for lithium metal anodes (LMAs) to enable uniform lithium deposition and enhance Li + flux. On one hand, the positively charged Ni 2+ sites in the polymer modify the electronic structure and provide robust electrostatic shielding to suppress adverse side reactions. On the other hand, the dense lithiophilic sites (C═N, C≡N, etc.) in HAT CN facilitate Li + diffusion and accelerate the desolvation process of Li + . Furthermore, the in‐depth working mechanisms behind these effects are revealed through a variety of in situ/ex situ characterizations and theoretical calculations. As a result, the Li + transference number of the Ni‐HAT CN‐protected battery increases to 0.76, and it exhibits stable cycling for over 3000 h (3 mA cm −2 ). The full cell maintains high capacity after 900 stable cycles at 1 C, with an average ultra‐low degradation rate of just 0.047% per cycle. This work offers a novel strategy for stabilizing LMAs by uniquely combining electrostatic field construction with the regulation of solvation structures.
Wu et al. (Fri,) studied this question.