In Situ Reformatsky Reaction‐Induced Surface Polymerization Toward an Oriented Monomeric Structure for Superior Zinc Anode Stability

ABSTRACT Addressing the intrinsic heterogeneity of zinc anodes, which triggers dendritic growth and parasitic reactions, is paramount for realizing safe and durable zinc‐ion batteries. The homogenization of in situ active sites and deposition serves as a critical approach to suppress dendrite growth. Herein, this work adopts an in situ Reformatsky reaction capable of eliminating active sites on the Zn surface while simultaneously generating a zincophilic metal‐organic polymer framework. This mechanism not only provides uniform ion channels but also promotes uniform zinc deposition by increasing the density of nucleation sites, ultimately inducing the preferential growth of thermodynamically stable (002) oriented zinc grains. As a result of this meticulously controlled interface, the protected zinc anode exhibits exceptional stability. The symmetrical battery can operate stably for 3,800 h at 1 mA cm −2 and even for more than 600 h at an ultra‐high current density of 10 mA cm −2 . More significantly, the resulting full cell achieves an ultra‐long lifespan exceeding 10,000 cycles at a current density of 5 A g −1 . This work demonstrates a highly effective strategy for practical zinc anodes while establishing a new design paradigm: controlling deposition kinetics through activation energy modulation for stable metal batteries.