Abstract Dendrite‐free Zn metal anodes with robust interface are highly desired for the practical application of aqueous zinc‐metal based batteries (AZMBs), while their stability is hindered by the untoward Zn(H 2 O) 6 2+ desolvation and succedent deposition with dissatisfactory kinetic barriers, especially under low‐temperature environment. Herein, a self‐cascade catalytic strategy on accelerating interfacial desolvation and optimizing diffusion is proposed by designing an atomically dispersed Bi within the deficient LaMnO 3.15 perovskite (SABi/U‐LMO) layer on Zn anode. Theoretical calculations demonstrate that the d ‐band center and nonbonding state near the Fermi level of SABi/U‐LMO alleviate the corrosion of H 2 O and accelerate the dissociation of Zn 2+ ─H 2 O bond by promoting the rapid filling of the empty 4s orbital of the Zn 2+ , as revealed by electrochemical and spectroscopic results. Meanwhile, the redistribution of electric field with SABi/U‐LMO realizes the delocalization and lateral growth of Zn atoms. Consequently, the cells with SABi/U‐LMO render an impressive lifetime up to 5000 h at 1 mA cm −2 as well as a high Coulombic efficiency of 99.59% over 2000 cycles under 0 °C. Full cell also stabilizes the capacity retention of ∼100% after 900 cycles at 1 A g −1 under −20 °C, verifying the feasibility of self‐cascade catalysis in realizing high‐performance AZMBs.
Cheng et al. (Mon,) studied this question.