Realizing High Reversible Zinc Metal Anode by Modulating Surface Chemistry and Crystal Structure

Abstract The uncontrollable dendrite growth on the Zn metal anode severely deteriorates the capacity and cycling stability of aqueous zinc–ion batteries (AZIBs), thereby retarding their practical application. In this work, through the combination of surface chemistry and crystal structure regulation, a duplex route of plasma sputtering and mechanical stretching is proposed to remove surface passivation layer and increase surface crystal defect (dislocations and textures) of Zn metal anode itself. Plasma sputtering can almost completely remove the surface passivation layer, ensuring a uniform Zn 2+ flux at the interface, which is conducive to uniform nucleation. Mechanical stretching can increase the surface dislocation density and (002) texture, the former can reduce Zn 2+ nucleation barrier, while the latter can guide Zn to grow parallel to the surface, inhibiting the growth of dendrites. Consequently, the as‐fabricated symmetrical cells exhibit stable and long lifespan (3560 h at 0.5 mA cm −2 for 0.5 mA h cm −2 ). The assembled full cells with α‐MnO 2 cathode deliver a nearly 100% average coulombic efficiency even after 1000 cycles at 5 A g −1 . Coupling a surface chemistry regulation with crystal structure control will be enlightening for solve the issues of metallic anodes in advanced metallic‐based batteries.