ABSTRACT The commercialization of lithium metal batteries (LMBs) is fundamentally challenged by Li dendrite growth, which originates from an unstable solid electrolyte interphase (SEI). Engineering a Li 3 N‐enriched SEI is highly desirable for achieving high conductivity and mechanical strength, but the kinetic barrier of the LiNO 3 ‐to‐Li 3 N conversion remains a major obstacle. Here, we report a catalytic approach to engineer Li 3 N‐enriched SEI layers by accelerating LiNO 3 reduction using transition metal single‐atom catalysts supported on nitrogen‐doped carbon (M/NC, M = Cr, Mn, Fe, Co, Ni, Zn). Among them, Co/NC exhibits the highest catalytic activity, leading to an SEI with significantly enhanced mechanical robustness and ionic transport. Theoretical calculations reveal that the superior performance of Co/NC stems from the minimal energy difference between its frontier molecular orbitals and those of the key LiNO intermediate, facilitating the electron transfer process. Consequently, the symmetric battery using Co/NC catalyst achieves exceptional cyclability for over 2500 h (1 mA cm −2 , 1 mAh cm −2 ). When applied in full cells, the Co/NC‐modified current collector also yields a dramatically prolonged cycle life. This work underscores the profound role of interfacial catalysis in designing high‐performance SEI for practical LMBs.
Sun et al. (Fri,) studied this question.