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Aqueous zinc‐iodine (Zn─I2) battery is a promising energy storage system due to its inherent safety, high theoretical capacity, sustainability, and cost‐effectiveness. However, the shuttle effect of polyiodide severely affects the stable loading of active iodine and even accelerates the corrosion of the Zn anode, thus impeding its further advancement. Herein, a unique trimethylsulfonium cation (TMS+) with strong adsorption is proposed to stabilize both the iodine cathode and Zn anode. Benefiting from the robust interaction between TMS+ and polyiodide, the electrolyte can effectively immobilize large‐capacity iodine in the form of oily precipitate, thus avoiding the shuttle effect of polyiodide and the Zn corrosion. Additionally, TMS+ can be preferentially adsorbed on various Zn facets, inducing an electrostatic shielding effect to inhibit Zn dendrite growth. Consequently, Zn anode can be stably cycled over 3400 h at 5 mA cm−2/5 mAh cm−2, and a large areal capacity of 2.71 mAh cm−2 as well as long‐life stability over 6400 cycles is achieved for Zn─I2 battery. Furthermore, cation adsorption engineering is practically utilized in pouch cells, realizing superior fast‐charging stability over 790 cycles. This electrolyte modification with dual stabilizations is anticipated to be applied to other metal‐iodine batteries as a cost‐effective, facile, and safe strategy. [ABSTRACT FROM AUTHOR]

• Cu@CuO nanowire arrays with facile scalability are proposed as protective layer for zinc anode. • The Zn2+ transport both in uniformity and transfer kinetics is comprehensively regulated by Cu@CuO nanowire arrays. • The assembled zinc anode with Cu@CuO nanowire arrays has significantly enhanced cycling stability in symmetric cells and pouch cells. Aqueous zinc (Zn) metal battery is regarded as a promising candidate with low cost and high safety for energy storage systems at large scales. However, the destabilized Zn2+ transport at the reaction interface severely restricts the lifespan of zinc anode, and the strategies suitable for large-scale integration of the anode's protection layer are required. Herein, an independent protective layer of Cu@CuO nanowire arrays is proposed to stabilize zinc anode with comprehensive regulation of Zn2+ transport. Through wet-chemical etching, the nanowire structure with a geometric area of 250 cm2 can be synthesized in one pot. From experimental analysis and simulation results, such a layer not only homogenizes the distribution of interfacial electric field, but also enhances Zn2+ transfer kinetics with improved ionic conductivity and increased transference number. Meanwhile, the activity of hydrogen evolution reaction (HER) is decreased due to the integration of this unique layer. As a result, the protected zinc anode can be stably operated at 2 mA cm−2/2 mAh cm−2, and the stable current density can further increase to 10 mA cm−2. Furthermore, the protective layer is featured with superior hydrophilicity, and can be feasibly utilized for large-area pouch cells, revealing the scalability and effectiveness in practical devices. This work proposes a facile protection strategy for zinc anode from the perspective of optimizing Zn2+ transport by large-scale integration of superior ion transport layer, showing great potential in high-performance zinc metal anode. [ABSTRACT FROM AUTHOR]

The work proposed a new insight into in situ construction of anti-corrosion structure via intermediate carbon cloth for long-life zinc anode, featuring the regulation of byproduct growth and the inhibition of HER. [Display omitted] • Intermediate carbon cloth undertook most of the anode reactions after activation. • The growth of ZHS byproduct on intermediate carbon cloth was effectively regulated. • The regulated ZHS byproduct in turn suppressed parasitic reaction. • Long cycling life was obtained for the incorporation of carbon cloth with Zn metal. Metallic zinc is regarded as an ideal anode in aqueous batteries, while the poor life associated with the ever-deepening interface corrosion and dendrite growth severely restricts the practical application. Herein, in situ construction of anti-corrosion structure via intermediate carbon cloth is developed to realize stable Zn deposition for long-life utilization. During the repeated charge and discharge, anode reactions including Zn plating and the parasitic reactions are gradually transferred to the intermediate carbon surface, and the growth of byproduct (zinc hydroxide sulfate, also ZHS) is regulated as a lateral pattern. This stable interface growth activates the stabilizing effect from ZHS and makes it an anti-corrosion structure for further Zn deposition. Meanwhile, such a layer also effectively adsorbs Zn atoms for the uniform nucleation and growth. As a result, over 3200 h of stable Zn plating/stripping is realized at a practical current density of 1 mA cm−2, and both the reaction current and the capacity can be stably extended to 10 mA cm−2 and 10 mAh cm−2. This work redefines the stabilizing effect of conductive interphase layer, and provides a new insight into the growth regulation of ZHS byproduct and the self anti-corrosion effect. [ABSTRACT FROM AUTHOR]