Zincophilic Porous Carbon Interface with Dendrite‐Free Zinc Deposition via Selective Ion Regulation for Aqueous Zinc Ion Batteries

ABSTRACT The development of a protective layer that not only blocks parasitic reactions but also actively regulates Zn 2+ transport and nucleation behavior is critical for the advancement of aqueous zinc‐ion batteries (AZIBs). In this study, we propose a novel interfacial engineering strategy based on a zincophilic porous carbon (ZPC) coating, which provided selective Zn 2+ adsorption and directional Zn 2+ flux regulation. The ZPC layer composed of poly (acrylic acid) (PAA)‐grafted carboxymethyl cellulose (CMC) (CLP) and activated carbon (AC) synergistically integrates zincophilic functional groups and a porous structure. This design enables rapid Zn 2+ desolvation and effectively suppresses dendrite formation. The selective Zn 2+ affinity of the ZPC layer minimizes hydrogen evolution reaction (HER) and corrosion, while promoting preferential Zn deposition along the (002) crystallographic plane. As a result, ZPC@Zn exhibits an extended lifespan exceeding 3600 h at 4 mA cm −2 and stable Zn plating/stripping at a high depth of discharge (DOD, 43%). Full cells paired with an iodine cathode demonstrate excellent rate capability and outstanding cycle stability, maintaining approximately 90% capacity retention over 5000 cycles at 10 C. This work establishes a new paradigm in interfacial layer design and paves the way for dendrite‐free, high‐performance AZIBs.