Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety, cost-effectiveness, and high capacity. However, the service life of zinc metal anodes is severely constrained by critical challenges, including dendrites, water-induced hydrogen evolution, and passivation. In this study, a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method. The ultrathin interphase layer (∼1 µm) is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1 Å, which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions, contributing to a uniform and highly reversible zinc deposition. With the shielding of the interphase layer, an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and ∼700 h at 1 mA cm−2, far exceeding that of the bare zinc anodes (250 and 70 h). Furthermore, as a proof-of-concept demonstration, the full cell paired with MnO2 cathode demonstrates improved rate performances and stable cycling (1200 cycles at 1 A g−1). This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.
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