Dynamic Restraining of Non‐(001) Planes via Incorporating Fe‐N‐C Nanoparticles Electrolyte Additive for Dendrite‐Free Zinc Metal Anodes

Abstract Aqueous zinc ion batteries have emerged as a promising alternative for high‐safety energy storage systems. However, in conventional configurations, Zn deposition often results in randomly orientated hexagonal platelets on the anode, leading to undesired dendrite growth and reduced battery lifespan. In this study, a dynamic regulation strategy is presented to promote (002)‐texture growth during Zn deposition. Single‐atomic iron‐decorated nitrogen‐carbon (Fe‐N‐C) nanoparticles, which can preferentially adsorb on Zn (100) and (101) planes during Zn deposition, are synthesized and incorporated into the electrolyte as an additive. Taking advantage of the reversible adsorption–desorption behavior of Fe‐N‐C agents, only the planar (002) plane of Zn remain exposed during battery cycling, effectively suppressing hydrogen evolution and dendrite formation. Consequently, Zn//Zn symmetry batteries with Fe‐N‐C electrolyte additive demonstrate an impressive cycling lifespan of 4,300 h with a cumulative plating capacity of 10.75 Ah cm ⁻² . Notably, even at a high depth of discharge of 61.5%, the batteries maintain remarkable cycling stability of 120 h. When paired with vanadium‐based oxide cathodes, full cells show outstanding durability, sustaining over 4,000 cycles with a capacitance retention of 91.7%. This study presents a simple yet effective strategy for constructing dendrite‐free electrode surfaces, advancing the development of stable Zn‐based energy storage devices.