Modulating Zinc Metal Reversibility by Confined Antifluctuator Film for Durable and Dendrite‐Free Zinc Ion Batteries

Abstract Aqueous Zn ion batteries are promising systems due to their intrinsic safety, low cost, and non‐toxicity, and the Zn corrosion and dendrite growth will cause the poor reversibility of Zn anode. Herein, the porous Zn@C solid, hollow, and yolk–shell microsphere films are developed as Zn anode antifluctuator (ZAAF). The prepared yolk–shell microspheres (Zn@C yolk–shell microsphere [ZCYSM]) film with superior buffering can effectively restrict the deposition of Zn metal in its interior and inhibit the volume expansion during plating/stripping process, thus modulating the Zn²⁺ flux and enabling stable Zn cycling. As a proof of concept, the ZCYSM@Zn symmetric cells achieve the excellent cyclic stability over 4000 h and cumulative plated capacity of 4 Ah cm⁻² at a high current density of 10 mA cm⁻². Concomitantly, the suppressed corrosion reactions and dendrite‐free ZAAF significantly improve the durability of full cells (coupled to CaV₆O₁₆·3H₂O). Additionally, durable pouch cell and electrochemical neuromorphic inorganic device (ENIDe) are integrated to simulate neural network, providing a strategy for extreme interconnectivity comparable to the human brain.